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Description
Lateral programmable metallization cells (PMC) utilize the properties of electrodeposits grown over a solid electrolyte channel. Such devices have an active anode and an inert cathode separated by a long electrodeposit channel in a coplanar arrangement. The ability to transport large amount of metallic mass across the channel makes these

Lateral programmable metallization cells (PMC) utilize the properties of electrodeposits grown over a solid electrolyte channel. Such devices have an active anode and an inert cathode separated by a long electrodeposit channel in a coplanar arrangement. The ability to transport large amount of metallic mass across the channel makes these devices attractive for various More-Than-Moore applications. Existing literature lacks a comprehensive study of electrodeposit growth kinetics in lateral PMCs. Moreover, the morphology of electrodeposit growth in larger, planar devices is also not understood. Despite the variety of applications, lateral PMCs are not embraced by the semiconductor industry due to incompatible materials and high operating voltages needed for such devices. In this work, a numerical model based on the basic processes in PMCs – cation drift and redox reactions – is proposed, and the effect of various materials parameters on the electrodeposit growth kinetics is reported. The morphology of the electrodeposit growth and kinetics of the electrodeposition process are also studied in devices based on Ag-Ge30Se70 materials system. It was observed that the electrodeposition process mainly consists of two regimes of growth – cation drift limited regime and mixed regime. The electrodeposition starts in cation drift limited regime at low electric fields and transitions into mixed regime as the field increases. The onset of mixed regime can be controlled by applied voltage which also affects the morphology of electrodeposit growth. The numerical model was then used to successfully predict the device kinetics and onset of mixed regime. The problem of materials incompatibility with semiconductor manufacturing was solved by proposing a novel device structure. A bilayer structure using semiconductor foundry friendly materials was suggested as a candidate for solid electrolyte. The bilayer structure consists of a low resistivity oxide shunt layer on top of a high resistivity ion carrying oxide layer. Devices using Cu2O as the low resistivity shunt on top of Cu doped WO3 oxide were fabricated. The bilayer devices provided orders of magnitude improvement in device performance in the context of operating voltage and switching time. Electrical and materials characterization revealed the structure of bilayers and the mechanism of electrodeposition in these devices.
ContributorsChamele, Ninad (Author) / Kozicki, Michael (Thesis advisor) / Barnaby, Hugh (Committee member) / Newman, Nathan (Committee member) / Gonzalez-Velo, Yago (Committee member) / Arizona State University (Publisher)
Created2020
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Description
The passivity of metals is a phenomenon of vast importance as it prevents many materials in important applications from rapid deterioration by corrosion. Alloying with a sufficient quantity of passivating elements (Cr, Al, Si), typically in the range of 10% - 20%, is commonly employed to improve the corrosion resistance

The passivity of metals is a phenomenon of vast importance as it prevents many materials in important applications from rapid deterioration by corrosion. Alloying with a sufficient quantity of passivating elements (Cr, Al, Si), typically in the range of 10% - 20%, is commonly employed to improve the corrosion resistance of elemental metals. However, the compositional criteria for enhanced corrosion resistance have been a long-standing unanswered question for alloys design. With the emerging interest in multi-principal element alloy design, a percolation model is developed herein for the initial stage of passive film formation, termed primary passivation. The successful validation of the assumptions and predictions of the model in three corrosion-resistant binary alloys, Fe-Cr, Ni-Cr, and Cu-Rh supports that the model which can be used to provide a quantitative design strategy for designing corrosion-resistant alloys. To date, this is the only model that can provide such criteria for alloy design.The model relates alloy passivation to site percolation of the passivating elements in the alloy matrix. In the initial passivation stage, Fe (Ni in Ni-Cr or Cu in Cu-Rh) is selectively dissolved, destroying the passive network built up by Cr (or Rh) oxides and undercutting isolated incipient Cr (Rh) oxide nuclei. The only way to prevent undercutting and form a stable protective passive film is if the concentration of Cr (Rh) is high enough to realize site percolation within the thickness of the passive film or the dissolution depth. This 2D-3D percolation cross-over transition explains the compositional dependent passivation of these alloys. The theoretical description of the transition and its assumptions is examined via experiments and kinetic Monte Carlo simulations. The initial passivation scenario of the dissolution selectivity is validated by the inductively coupled plasma mass spectrum (ICP-MS). The electronic effect not considered in the kinetic Monte Carlo simulations is addressed by density functional theory (DFT). Additionally, the impact of the atomic configuration parameter on alloy passivation is experimentally measured, which turns out to agree well with the model predictions developed using Monte Carlo renormalization group (MC-RNG) methods.
ContributorsXie, Yusi (Author) / Sieradzki, Karl KS (Thesis advisor) / Chan, Candace CC (Committee member) / Wang, Qing QHW (Committee member) / Buttry, Daniel DB (Committee member) / Arizona State University (Publisher)
Created2020
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Description
The origins of carrier mobility (μe) were thoroughly investigated in hydrogenated indium oxide (IO:H) and zinc-tin oxide (ZTO) transparent conducting oxide (TCO) thin films. A carrier transport model was developed for IO:H which studied the effects of ionized impurity scattering, polar optical phonon scattering, and grain boundary scattering. Ionized impurity

The origins of carrier mobility (μe) were thoroughly investigated in hydrogenated indium oxide (IO:H) and zinc-tin oxide (ZTO) transparent conducting oxide (TCO) thin films. A carrier transport model was developed for IO:H which studied the effects of ionized impurity scattering, polar optical phonon scattering, and grain boundary scattering. Ionized impurity scattering dominated at temperatures below ~240 K. A reduction in scattering charge Z from +2 to +1 as atomic %H increased from ~3 atomic %H to ~5 atomic %H allowed μe to attain >100 cm^2/Vs at ~5 atomic %H.

In highly hydrogenated IO:H, ne significantly decreased as temperature increased from 5 K to 140 K. To probe this unusual behavior, samples were illuminated, then ne, surface work function (WF), and spatially resolved microscopic current mapping were measured and tracked. Large increases in ne and corresponding decreases in WF were observed---these both exhibited slow reversions toward pre-illumination values over 6-12 days. A hydrogen-related defect was proposed as source of the photoexcitation, while a lattice defect diffusion mechanism causes the extended decay. Both arise from an under-coordination of the In.

An enhancement of μe was observed with increasing amorphous fraction in IO:H. An increase in population of corner- and edge-sharing polyhedra consisting of metal cations and oxygen anions is thought to be the origin. This indicates some measure of medium-range order in the amorphous structure, and gives rise to a general principle dictating μe in TCOs---even amorphous TCOs. Testing this principle resulted in observing an enhancement of μe up to 35 cm^2/Vs in amorphous ZTO (a-ZTO), one of the highest reported a-ZTO μe values (at ne > 10^19 cm^-3) to date. These results highlight the role of local distortions and cation coordination in determining the microscopic origins of carrier generation and transport. In addition, the strong likelihood of under-coordination of one cation species leading to high carrier concentrations is proposed. This diverges from the historical indictment of oxygen vacancies controlling carrier population in crystalline oxides, which by definition cannot occur in amorphous systems, and provides a framework to discuss key structural descriptors in these disordered phase materials.
ContributorsHusein, Sebastian S.T. (Author) / Bertoni, Mariana I. (Thesis advisor) / Stuckelberger, Michael (Committee member) / Holman, Zachary C. (Committee member) / Crozier, Peter (Committee member) / Arizona State University (Publisher)
Created2020
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Description
In the current photovoltaic (PV) industry, the O&M (operations and maintenance) personnel in the field primarily utilize three approaches to identify the underperforming or defective modules in a string: i) EL (electroluminescence) imaging of all the modules in the string; ii) IR (infrared) thermal imaging of all the modules in

In the current photovoltaic (PV) industry, the O&M (operations and maintenance) personnel in the field primarily utilize three approaches to identify the underperforming or defective modules in a string: i) EL (electroluminescence) imaging of all the modules in the string; ii) IR (infrared) thermal imaging of all the modules in the string; and, iii) current-voltage (I-V) curve tracing of all the modules in the string. In the first and second approaches, the EL images are used to detect the modules with broken cells, and the IR images are used to detect the modules with hotspot cells, respectively. These two methods may identify the modules with defective cells only semi-qualitatively, but not accurately and quantitatively. The third method, I-V curve tracing, is a quantitative method to identify the underperforming modules in a string, but it is an extremely time consuming, labor-intensive, and highly ambient conditions dependent method. Since the I-V curves of individual modules in a string are obtained by disconnecting them individually at different irradiance levels, module operating temperatures, angle of incidences (AOI) and air-masses/spectra, all these measured curves are required to be translated to a single reporting condition (SRC) of a single irradiance, single temperature, single AOI and single spectrum. These translations are not only time consuming but are also prone to inaccuracy due to inherent issues in the translation models. Therefore, the current challenges in using the traditional I-V tracers are related to: i) obtaining I-V curves simultaneously of all the modules and substrings in a string at a single irradiance, operating temperature, irradiance spectrum and angle of incidence due to changing weather parameters and sun positions during the measurements, ii) safety of field personnel when disconnecting and reconnecting of cables in high voltage systems (especially field aged connectors), and iii) enormous time and hardship for the test personnel in harsh outdoor climatic conditions. In this thesis work, a non-contact I-V (NCIV) curve tracing tool has been integrated and implemented to address the above mentioned three challenges of the traditional I-V tracers.

This work compares I-V curves obtained using a traditional I-V curve tracer with the I-V curves obtained using a NCIV curve tracer for the string, substring and individual modules of crystalline silicon (c-Si) and cadmium telluride (CdTe) technologies. The NCIV curve tracer equipment used in this study was integrated using three commercially available components: non-contact voltmeters (NCV) with voltage probes to measure the voltages of substrings/modules in a string, a hall sensor to measure the string current and a DAS (data acquisition system) for simultaneous collection of the voltage data obtained from the NCVs and the current data obtained from the hall sensor. This study demonstrates the concept and accuracy of the NCIV curve tracer by comparing the I-V curves obtained using a traditional capacitor-based tracer and the NCIV curve tracer in a three-module string of c-Si modules and of CdTe modules under natural sunlight with uniform light conditions on all the modules in the string and with partially shading one or more of the modules in the string to simulate and quantitatively detect the underperforming module(s) in a string.
ContributorsMurali, Sanjay (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Srinivasan, Devarajan (Committee member) / Rogers, Bradley (Committee member) / Arizona State University (Publisher)
Created2020
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Description

Bio-modification of asphalt binder brings significant benefits in terms of increasing sustainable and environmental practices, stabilizing prices, and decreasing costs. However, bio-modified asphalt binders have shown varying performance regarding susceptibility to moisture damage; some bio-oil modifiers significantly increase asphalt binder's susceptibility to moisture damage. This variability in performance is largely

Bio-modification of asphalt binder brings significant benefits in terms of increasing sustainable and environmental practices, stabilizing prices, and decreasing costs. However, bio-modified asphalt binders have shown varying performance regarding susceptibility to moisture damage; some bio-oil modifiers significantly increase asphalt binder's susceptibility to moisture damage. This variability in performance is largely due to the large number of bio-masses available for use as sources of bio-oil, as well as the type of processing procedure followed in converting the bio-mass into a bio-oil for modifying asphalt binder. Therefore, there is a need for a method of properly evaluating the potential impact of a bio-oil modifier for asphalt binder on the overall performance of asphalt pavement, in order to properly distinguish whether a particular bio-oil modifier increases or decreases the moisture susceptibility of asphalt binder. Therefore, the goal of this study is a multi-scale investigation of bio-oils with known chemical compositions to determine if there is a correlation between a fundamental property of a bio-oil and the resulting increase or decrease in moisture susceptibility of a binder when it is modified with the bio-oil. For instance, it was found that polarizability of asphalt constituents can be a promising indicator of moisture susceptibility of bitumen. This study will also evaluate the linkage of the fundamental property to newly developed binder-level test methods. It was found that moisture-induced shear thinning of bitumen containing glass beads can differentiate moisture susceptible bitumen samples. Based on the knowledge determined, alternative methods of reducing the moisture susceptibility of asphalt pavement will also be evaluated. It was shown that accumulation of acidic compounds at the interface of bitumen and aggregate could promote moisture damage. It was further found that detracting acidic compounds from the interface could be done by either of neutralizing active site of stone aggregate to reduce affinity for acids or by arresting acidic compounds using active mineral filler. The study results showed there is a strong relation between composition of bitumen and its susceptibility to moisture. This in turn emphasize the importance of integrating knowledge of surface chemistry and bitumen composition into the pavement design and evaluation.

ContributorsOldham, Daniel Joshua (Author) / Fini, Elham F (Thesis advisor) / Kaloush, Kamil (Committee member) / Deng, Shuguang (Committee member) / Mallick, Rajib B (Committee member) / Louie, Stacey M (Committee member) / Parast, Mahour M (Committee member) / Arizona State University (Publisher)
Created2020
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Description
Metal-organic frameworks have made a feature in the cutting-edge technology with a wide variety of applications because they are the new material candidate as adsorbent or membrane with high surface area, various pore sizes, and highly tunable framework functionality properties. The emergence of two-dimensional (2D) metal-organic frameworks has surged an

Metal-organic frameworks have made a feature in the cutting-edge technology with a wide variety of applications because they are the new material candidate as adsorbent or membrane with high surface area, various pore sizes, and highly tunable framework functionality properties. The emergence of two-dimensional (2D) metal-organic frameworks has surged an outburst of intense research to understand the feasible synthesis and exciting material properties of these class of materials. Despite their potential, studies to date show that it is extremely challenging to synthesize and manufacture 2D MOF at large scales with ultimate control over crystallinity and thickness.

The field of research to date has produced various synthesis routes which can further be used to design 2D materials with a range of organic ligands and metal linkers. This thesis seeks to extend these design rules to demonstrate the competitive growth of two- dimensional (2D) metal-organic frameworks(MOF) and their alloys to predict which ligands and metals can be combined, study the intercalation of Bromine in these frameworks and their alloys which leads to the discovery of reduced band gap in the layered MOF alloy.

In this study it has been shown that the key factor in achieving layered 2D MOFs and it relies on the use of carefully engineered ligands to terminate the out-of-plane sites on metal clusters thereby eliminating strong interlayer hydrogen bond formation.

The major contribution of pyridine is to replace interlayer hydrogen bonding or other weak chemical bonds. Overall results establish an entirely new synthesis method for producing highly crystalline and scalable 2D MOFs and their alloys. Bromine intercalation merits future studies on band gap engineering in these layered materials.
ContributorsVijay, Shiljashree (Author) / Tongay, Sefaattin (Thesis advisor) / Green, Matthew D (Committee member) / Zhuang, Houlong (Committee member) / Arizona State University (Publisher)
Created2020
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Description
The main objective of this research is to develop reliability assessment methodologies to quantify the effect of various environmental factors on photovoltaic (PV) module performance degradation. The manufacturers of these photovoltaic modules typically provide a warranty level of about 25 years for 20% power degradation from the initial specified power

The main objective of this research is to develop reliability assessment methodologies to quantify the effect of various environmental factors on photovoltaic (PV) module performance degradation. The manufacturers of these photovoltaic modules typically provide a warranty level of about 25 years for 20% power degradation from the initial specified power rating. To quantify the reliability of such PV modules, the Accelerated Life Testing (ALT) plays an important role. But there are several obstacles that needs to be tackled to conduct such experiments, since there has not been enough historical field data available. Even if some time-series performance data of maximum output power (Pmax) is available, it may not be useful to develop failure/degradation mode-specific accelerated tests. This is because, to study the specific failure modes, it is essential to use failure mode-specific performance variable (like short circuit current, open circuit voltage or fill factor) that is directly affected by the failure mode, instead of overall power which would be affected by one or more of the performance variables. Hence, to address several of the above-mentioned issues, this research is divided into three phases. The first phase deals with developing models to study climate specific failure modes using failure mode specific parameters instead of power degradation. The limited field data collected after a long time (say 18-21 years), is utilized to model the degradation rate and the developed model is then calibrated to account for several unknown environmental effects using the available qualification testing data. The second phase discusses the cumulative damage modeling method to quantify the effects of various environmental variables on the overall power production of the photovoltaic module. Mainly, this cumulative degradation modeling approach is used to model the power degradation path and quantify the effects of high frequency multiple environmental input data (like temperature, humidity measured every minute or hour) with very sparse response data (power measurements taken quarterly or annually). The third phase deals with optimal planning and inference framework using Iterative-Accelerated Life Testing (I-ALT) methodology. All the proposed methodologies are demonstrated and validated using appropriate case studies.
ContributorsBala Subramaniyan, Arun (Author) / Pan, Rong (Thesis advisor) / Tamizhmani, Govindasamy (Thesis advisor) / Montgomery, Douglas C. (Committee member) / Wu, Teresa (Committee member) / Kuitche, Joseph (Committee member) / Arizona State University (Publisher)
Created2020
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Description
Vibrational spectroscopy is a ubiquitous characterization tool in elucidating atomic structure at the bulk and nanoscale. The ability to perform high spatial resolution vibrational spectroscopy in a scanning transmission electron microscope (STEM) with electron energy-loss spectroscopy (EELS) has the potential to affect a variety of materials science problems. Since 2014,

Vibrational spectroscopy is a ubiquitous characterization tool in elucidating atomic structure at the bulk and nanoscale. The ability to perform high spatial resolution vibrational spectroscopy in a scanning transmission electron microscope (STEM) with electron energy-loss spectroscopy (EELS) has the potential to affect a variety of materials science problems. Since 2014, instrumentation development has pushed for incremental improvements in energy resolution, with the current best being 4.2 meV. Although this is poor in comparison to what is common in photon or neutron vibrational spectroscopies, the spatial resolution offered by vibrational EELS is equal to or better than the best of these other techniques.

The major objective of this research program is to investigate the spatial resolution of the monochromated energy-loss signal in the transmission-beam mode and correlate it to the excitation mechanism of the associated vibrational mode. The spatial variation of dipole vibrational signals in SiO2 is investigated as the electron probe is scanned across an atomically abrupt SiO2/Si interface. The Si-O bond stretch signal has a spatial resolution of 2 – 20 nm, depending on whether the interface, bulk, or surface contribution is chosen. For typical TEM specimen thicknesses, coupled surface modes contribute strongly to the spectrum. These coupled surface modes are phonon polaritons, whose intensity and spectral positions are strongly specimen geometry dependent. In a SiO2 thin-film patterned with a 2x2 array, dielectric theory simulations predict the simultaneous excitation of parallel and uncoupled surface polaritons and a very weak excitation of the orthogonal polariton.

It is demonstrated that atomic resolution can be achieved with impact vibrational signals from optical and acoustic phonons in a covalently bonded material like Si. Sub-nanometer resolution mapping of the Si-O symmetric bond stretch impact signal can also be performed in an ionic material like SiO2. The visibility of impact energy-loss signals from excitation of Brillouin zone boundary vibrational modes in hexagonal BN is seen to be a strong function of probe convergence, but not as strong a function of spectrometer collection angles. Some preliminary measurements to detect adsorbates on catalyst nanoparticle surfaces with minimum radiation damage in the aloof-beam mode are also presented.
ContributorsVenkatraman, Kartik (Author) / Crozier, Peter (Thesis advisor) / Rez, Peter (Committee member) / Wang, Robert (Committee member) / Tongay, Sefaattin (Committee member) / Arizona State University (Publisher)
Created2020
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Description
This dissertation covers my doctoral research on the cathodoluminescence (CL) study of the optical properties of III-niride semiconductors.

The first part of this thesis focuses on the optical properties of Mg-doped gallium nitride (GaN:Mg) epitaxial films. GaN is an emerging material for power electronics, especially for high power and high

This dissertation covers my doctoral research on the cathodoluminescence (CL) study of the optical properties of III-niride semiconductors.

The first part of this thesis focuses on the optical properties of Mg-doped gallium nitride (GaN:Mg) epitaxial films. GaN is an emerging material for power electronics, especially for high power and high frequency applications. Compared to traditional Si-based devices, GaN-based devices offer superior breakdown properties, faster switching speed, and reduced system size. Some of the current device designs involve lateral p-n junctions which require selective-area doping. Dopant distribution in the selectively-doped regions is a critical issue that can impact the device performance. While most studies on Mg doping in GaN have been reported for epitaxial grown on flat c-plane substrates, questions arise regarding the Mg doping efficiency and uniformity in selectively-doped regions, where growth on surfaces etched away from the exact c-plane orientation is involved. Characterization of doping concentration distribution in lateral structures using secondary ion mass spectroscopy lacks the required spatial resolution. In this work, visualization of acceptor distribution in GaN:Mg epilayers grown by metalorganic chemical vapor deposition (MOCVD) was achieved at sub-micron scale using CL imaging. This was enabled by establishing a correlation among the luminescence characteristics, acceptor concentration, and electrical conductivity of GaN:Mg epilayers. Non-uniformity in acceptor distribution has been observed in epilayers grown on mesa structures and on miscut substrates. It is shown that non-basal-plane surfaces, such as mesa sidewalls and surface step clusters, promotes lateral growth along the GaN basal planes with a reduced Mg doping efficiency. The influence of surface morphology on the Mg doping efficiency in GaN has been studied.

The second part of this thesis focuses on the optical properties of InGaN for photovoltaic applications. The effects of thermal annealing and low energy electron beam irradiation (LEEBI) on the optical properties of MOCVD-grown In0.14Ga0.86N films were studied. A multi-fold increase in luminescence intensity was observed after 800 °C thermal annealing or LEEBI treatment. The mechanism leading to the luminescence intensity increase has been discussed. This study shows procedures that significantly improve the luminescence efficiency of InGaN, which is important for InGaN-based optoelectronic devices.
ContributorsLiu, Hanxiao (Author) / Ponce, Fernando A. (Thesis advisor) / Zhao, Yuji (Committee member) / Newman, Nathan (Committee member) / Fischer, Alec M (Committee member) / Arizona State University (Publisher)
Created2020
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Description

This research is a comprehensive study of the sustainable modifiers for asphalt binder. It is a common practice to use modifiers to impart certain properties to asphalt binder; however, in order to facilitate the synthesis and design of highly effective sustainable modifiers, it is critical to thoroughly understand their underlying

This research is a comprehensive study of the sustainable modifiers for asphalt binder. It is a common practice to use modifiers to impart certain properties to asphalt binder; however, in order to facilitate the synthesis and design of highly effective sustainable modifiers, it is critical to thoroughly understand their underlying molecular level mechanisms in combination with micro and macro-level behavior. Therefore, this study incorporates a multi-scale approach using computational modeling and laboratory experiments to provide an in-depth understanding of the mechanisms of interaction between selected modifiers and the constituents of asphalt binder, at aged and unaged conditions. This study investigated the effect of paraffinic wax as a modifier for virgin binder in warm-mix asphalt that can reduce the environmental burden of asphalt pavements. The addition of wax was shown to reduce the viscosity of bitumen by reducing the self-interaction of asphaltene molecules and penetrating the existing nano agglomerates of asphaltenes. This study further examined how the interplay of various modifiers affects the modified binder’s thermomechanical properties. It was found that the presence of wax-based modifiers has a disrupting effect on the role of polyphosphoric acid that is another modifier of bitumen and its interactions with resin-type molecules.

This study was further extended to using nanozeolite as a mineral carrier for wax to better disperse wax in bitumen and reduce the wax's adverse effects such as physical hardening at low service temperatures and rutting at high service temperatures. This novel technique showed that using a different method of adding a modifier can help reduce the modifier's unwanted effects. It further showed that nanozeolite could carry wax-based modifiers and release them in bitumen, then acting as a scavenger for acidic compounds in the binder. This, in turn, could promote the resistance of asphalt binder to moisture damage by reducing the quantity of acidic compounds at the interface between the binder and the stone aggregates.

Furthermore, this study shows that iso-paraffin wax can reduce oxidized asphaltene molecules self-interaction and therefore, reduce the viscosity of aged bitumen while cause brittleness at low temperatures.

Additionally, a cradle to gate life-cycle assessment was performed for a new bio-modifier obtained from swine manure. This study showed that by partially replacing the bitumen with bio-binder from swine manure, the carbon footprint of the binder can be reduced by 10% in conjunction with reducing the cost and environmental impact of storing the manure in lagoons.

ContributorsSamieadel, Alireza (Author) / Fini, Elham H (Thesis advisor) / Kaloush, Kamil (Committee member) / Parrish, Kristen (Committee member) / Sharma, Brajendra Kumar (Committee member) / Parast, Mahour M (Committee member) / Arizona State University (Publisher)
Created2020