Matching Items (64)
Description
This dissertation will investigate two of the most promising high-capacity anode
materials for lithium-based batteries: silicon (Si) and metal lithium (Li). It will focus on
studying the mechanical behaviors of the two materials during charge and discharge and
understanding how these mechanical behaviors may affect their electrochemical
performance.
In the first part, amorphous Si anode will be studied. Despite many existing studies
on silicon (Si) anodes for lithium ion batteries (LIBs), many essential questions still exist
on compound formation, composition, and properties. Here it is shown that some
previously accepted findings do not truthfully reflect the actual lithiation mechanisms in
realistic battery configurations. Furthermore the correlation between structure and
mechanical properties in these materials has not been properly established. Here, a rigorous
and thorough study is performed to comprehensively understand the electrochemical
reaction mechanisms of amorphous-Si (a-Si) in a realistic LIB configuration. In-depth
microstructural characterization was performed and correlations were established between
Li-Si composition, volumetric expansion, and modulus/hardness. It is found that the
lithiation process of a-Si in a real battery setup is a single-phase reaction rather than the
accepted two-phase reaction obtained from in-situ TEM experiments. The findings in this
dissertation establish a reference to quantitatively explain many key metrics for lithiated a
Si as anodes in real LIBs, and can be used to rationally design a-Si based high-performance
LIBs guided by high-fidelity modeling and simulations.
In the second part, Li metal anode will be investigated. Problems related to dendrite
growth on lithium metal anodes such as capacity loss and short circuit present major
barriers to the next-generation high-energy-density batteries. The development of
successful mitigation strategies is impeded by the incomplete understanding of the Li
dendrite growth mechanisms. Here the enabling role of plating residual stress in dendrite
initiation through novel experiments of Li electrodeposition on soft substrates is confirmed,
and the observations is explained with a stress-driven dendrite growth model. Dendrite
growth is mitigated on such soft substrates through surface-wrinkling-induced stress
relaxation in deposited Li film. It is demonstrated that this new dendrite mitigation
mechanism can be utilized synergistically with other existing approaches in the form of
three-dimensional (3D) soft scaffolds for Li plating, which achieves superior coulombic
efficiency over conventional hard copper current collectors under large current density.
materials for lithium-based batteries: silicon (Si) and metal lithium (Li). It will focus on
studying the mechanical behaviors of the two materials during charge and discharge and
understanding how these mechanical behaviors may affect their electrochemical
performance.
In the first part, amorphous Si anode will be studied. Despite many existing studies
on silicon (Si) anodes for lithium ion batteries (LIBs), many essential questions still exist
on compound formation, composition, and properties. Here it is shown that some
previously accepted findings do not truthfully reflect the actual lithiation mechanisms in
realistic battery configurations. Furthermore the correlation between structure and
mechanical properties in these materials has not been properly established. Here, a rigorous
and thorough study is performed to comprehensively understand the electrochemical
reaction mechanisms of amorphous-Si (a-Si) in a realistic LIB configuration. In-depth
microstructural characterization was performed and correlations were established between
Li-Si composition, volumetric expansion, and modulus/hardness. It is found that the
lithiation process of a-Si in a real battery setup is a single-phase reaction rather than the
accepted two-phase reaction obtained from in-situ TEM experiments. The findings in this
dissertation establish a reference to quantitatively explain many key metrics for lithiated a
Si as anodes in real LIBs, and can be used to rationally design a-Si based high-performance
LIBs guided by high-fidelity modeling and simulations.
In the second part, Li metal anode will be investigated. Problems related to dendrite
growth on lithium metal anodes such as capacity loss and short circuit present major
barriers to the next-generation high-energy-density batteries. The development of
successful mitigation strategies is impeded by the incomplete understanding of the Li
dendrite growth mechanisms. Here the enabling role of plating residual stress in dendrite
initiation through novel experiments of Li electrodeposition on soft substrates is confirmed,
and the observations is explained with a stress-driven dendrite growth model. Dendrite
growth is mitigated on such soft substrates through surface-wrinkling-induced stress
relaxation in deposited Li film. It is demonstrated that this new dendrite mitigation
mechanism can be utilized synergistically with other existing approaches in the form of
three-dimensional (3D) soft scaffolds for Li plating, which achieves superior coulombic
efficiency over conventional hard copper current collectors under large current density.
ContributorsWang, Xu (Author) / Jiang, Hanqing (Thesis advisor) / Yu, Hongbin (Thesis advisor) / Chan, Candace (Committee member) / Wang, Liping (Committee member) / Qiong, Nian (Committee member) / Arizona State University (Publisher)
Created2018
Description
This work demonstrates a capable reverse pulse deposition methodology to influence gap fill behavior inside microvia along with a uniform deposit in the fine line patterned regions for substrate packaging applications. Interconnect circuitry in IC substrate packages comprises of stacked microvia that varies in depth from 20µm to 100µm with an aspect ratio of 0.5 to 1.5 and fine line patterns defined by photolithography. Photolithography defined pattern regions incorporate a wide variety of feature sizes including large circular pad structures with diameter of 20µm - 200µm, fine traces with varying widths of 3µm - 30µm and additional planar regions to define a IC substrate package. Electrodeposition of copper is performed to establish the desired circuit. Electrodeposition of copper in IC substrate applications holds certain unique challenges in that they require a low cost manufacturing process that enables a void-free gap fill inside the microvia along with uniform deposition of copper on exposed patterned regions. Deposition time scales to establish the desired metal thickness for such packages could range from several minutes to few hours. This work showcases a reverse pulse electrodeposition methodology that achieves void-free gap fill inside the microvia and uniform plating in FLS (Fine Lines and Spaces) regions with significantly higher deposition rates than traditional approaches. In order to achieve this capability, systematic experimental and simulation studies were performed. A strong correlation of independent parameters that govern the electrodeposition process such as bath temperature, reverse pulse plating parameters and the ratio of electrolyte concentrations is shown to the deposition kinetics and deposition uniformity in fine patterned regions and gap fill rate inside the microvia. Additionally, insight into the physics of via fill process is presented with secondary and tertiary current simulation efforts. Such efforts lead to show “smart” control of deposition rate at the top and bottom of via to avoid void formation. Finally, a parametric effect on grain size and the ensuing copper metallurgical characteristics of bulk copper is also shown to enable high reliability substrate packages for the IC packaging industry.
ContributorsGanesan, Kousik (Author) / Tasooji, Amaneh (Thesis advisor) / Manepalli, Rahul (Committee member) / Alford, Terry (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2018
In-situ photoemission spectroscopy characterization of electronic states in semiconductor interfaces
Description
The electronic states of semiconductor interfaces have significant importance for semiconductor device performance, especially due to the continuing miniaturization of device technology.
The application of ultra high vacuum (UHV) enables the preparation and characterization of fresh and cleaned interfaces. In a UHV environment, photoemission spectroscopy (PES) provides a non-destructive method to measure the electronic band structure, which is a crucial component of interface properties.
In this dissertation, three semiconductor interfaces were studies to understand different effects on electronic states. The interfaces studied were freshly grown or pre-treated under UHV. Then in-situ PES measurements, including x-ray photoemission spectroscopy (XPS) and ultra-violet photoemission spectroscopy (UPS), were conducted to obtain electronic states information.
First, the CdTe/InSb (100) heterointerface was employed as a model interface for II-VI and III-V heterojunctions. It was suggested that an interface layer formed, which consisted of In-Te bonding. The non-octal bonding between In and Te atoms has donor-like behavior, which was proposed to result in an electron accumulation layer in InSb. A type-I heterointerface was observed. Second, Cu/ZnO interfaces were studied to understand the interface bonding and the role of polarization on ZnO interfaces. It was shown that on O-face ZnO (0001) and PEALD ZnO, copper contacts had ohmic behavior. However, on Zn-face ZnO (0001), a 0.3 eV Schottky barrier height was observed. The lower than expected barrier heights were attributed to oxygen vacancies introduced by Cu-O bonding during interface formation. In addition, it is suggested that the different barrier heights on two sides of ZnO (0001) are caused by the different behavior for the ZnO (0001) faces. Last, a pulse mode deposition method was applied for P-doped diamond growth on (100) diamond surfaces. Pretreatment effects were studied. It is suggested that an O/H plasma treatment or a short period of H-plasma and CH4/H2 plasma could yield a higher growth rate. PES measurements were conducted on H-terminated intrinsic diamond surface and P-doped/intrinsic diamond (100) interfaces. It was suggested that electronic states near the valence band maximum caused Fermi level pinning effects, independent of the diamond doping.
The application of ultra high vacuum (UHV) enables the preparation and characterization of fresh and cleaned interfaces. In a UHV environment, photoemission spectroscopy (PES) provides a non-destructive method to measure the electronic band structure, which is a crucial component of interface properties.
In this dissertation, three semiconductor interfaces were studies to understand different effects on electronic states. The interfaces studied were freshly grown or pre-treated under UHV. Then in-situ PES measurements, including x-ray photoemission spectroscopy (XPS) and ultra-violet photoemission spectroscopy (UPS), were conducted to obtain electronic states information.
First, the CdTe/InSb (100) heterointerface was employed as a model interface for II-VI and III-V heterojunctions. It was suggested that an interface layer formed, which consisted of In-Te bonding. The non-octal bonding between In and Te atoms has donor-like behavior, which was proposed to result in an electron accumulation layer in InSb. A type-I heterointerface was observed. Second, Cu/ZnO interfaces were studied to understand the interface bonding and the role of polarization on ZnO interfaces. It was shown that on O-face ZnO (0001) and PEALD ZnO, copper contacts had ohmic behavior. However, on Zn-face ZnO (0001), a 0.3 eV Schottky barrier height was observed. The lower than expected barrier heights were attributed to oxygen vacancies introduced by Cu-O bonding during interface formation. In addition, it is suggested that the different barrier heights on two sides of ZnO (0001) are caused by the different behavior for the ZnO (0001) faces. Last, a pulse mode deposition method was applied for P-doped diamond growth on (100) diamond surfaces. Pretreatment effects were studied. It is suggested that an O/H plasma treatment or a short period of H-plasma and CH4/H2 plasma could yield a higher growth rate. PES measurements were conducted on H-terminated intrinsic diamond surface and P-doped/intrinsic diamond (100) interfaces. It was suggested that electronic states near the valence band maximum caused Fermi level pinning effects, independent of the diamond doping.
ContributorsWang, Xingye (Author) / Nemanich, Robert J (Thesis advisor) / Chan, Candace (Committee member) / Ponce, Fernando (Committee member) / Holman, Zachary (Committee member) / Arizona State University (Publisher)
Created2018
Description
Polycrystalline magnetite thin films were deposited on large area polymer substrates using aqueous solution based spin-spray deposition (SSD). This technique involved the hydrolysis of precursor salt solutions at low temperatures (70-100°C). The fundamental mechanisms and pathways in crystallization and evolution of the film microstructures were studied as a function of reactant chemistry and reactor conditions (rotation rate, flow rates etc.). A key feature of this method was the ability to constantly supply fresh solutions throughout deposition. Solution flow due to substrate rotation ensured that reactant depleted solutions were spun off. This imparted a limited volume, near two-dimensional restriction on the growth process. Film microstructure was studied as a function of process parameters such as liquid flow rate, nebulizer configuration, platen rotation rate and solution chemistry. It was found that operating in the micro-droplet regime of deposition was a crucial factor in controlling the microstructure.
Film porosity and substrate adhesion were linked to the deposition rate, which in-turn depended on solution chemistry. Films exhibited a wide variety of hierarchically organized microstructures often spanning length scales from tens-of-nanometers to a few microns. These included anisotropic morphologies such as nanoplates and nanoblades, that were generally unexpected from magnetite (a high symmetry cubic solid). Time resolved studies showed that the reason for complex hierarchy in microstructure was the crystallization via non-classical pathways. SSD of magnetite films involved formation of precursor phases that subsequently underwent solid-state transformations and nanoparticle self-assembly. These precursor phases were identified and possible reaction mechanisms for the formation of magnetite were proposed. A qualitative description of the driving forces for self-assembly was presented.
Film porosity and substrate adhesion were linked to the deposition rate, which in-turn depended on solution chemistry. Films exhibited a wide variety of hierarchically organized microstructures often spanning length scales from tens-of-nanometers to a few microns. These included anisotropic morphologies such as nanoplates and nanoblades, that were generally unexpected from magnetite (a high symmetry cubic solid). Time resolved studies showed that the reason for complex hierarchy in microstructure was the crystallization via non-classical pathways. SSD of magnetite films involved formation of precursor phases that subsequently underwent solid-state transformations and nanoparticle self-assembly. These precursor phases were identified and possible reaction mechanisms for the formation of magnetite were proposed. A qualitative description of the driving forces for self-assembly was presented.
ContributorsVadari Venkata, Kaushik Sridhar (Author) / Petuskey, William (Thesis advisor) / Carpenter, Ray (Committee member) / McCartney, Martha (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2018
Description
Two-dimensional transition metal dichalcogenides (TMDCs) such as
molybdenum disulfide (MoS2), tungsten disulfide (WS2), molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2) are attractive for use in biotechnology, optical and electronics devices due to their promising and tunable electrical, optical and chemical properties. To fulfill the variety of requirements for different applications, chemical treatment methods are developed to tune their properties. In this dissertation, plasma treatment, chemical doping and functionalization methods have been applied to tune the properties of TMDCs. First, plasma treatment of TMDCs results in doping and generation of defects, as well as the synthesis of transition metal oxides (TMOs) with rolled layers that have increased surface-to-volume ratio and are promising for electrochemical applications. Second, chemical functionalization is another powerful approach for tuning the properties of TMDCs for use in many applications. To covalently functionalize the basal planes of TMDCs, previous reports begin with harsh treatments like lithium intercalation that disrupt the structure and lead to a phase transformation from semiconducting to metallic. Instead, this work demonstrates the direct covalent functionalization of semiconducting MoS2 using aryl diazonium salts without lithium treatments. It preserves the structure and semiconducting nature of MoS2, results in covalent C-S bonds on basal planes and enables different functional groups to be tethered to the MoS2 surface via the diazonium salts. The attachment of fluorescent proteins has been used as a demonstration and it suggests future applications in biology and biosensing. The effects of the covalent functionalization on the electronic transport properties of MoS2 were then studied using field effect transistor (FET) devices.
molybdenum disulfide (MoS2), tungsten disulfide (WS2), molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2) are attractive for use in biotechnology, optical and electronics devices due to their promising and tunable electrical, optical and chemical properties. To fulfill the variety of requirements for different applications, chemical treatment methods are developed to tune their properties. In this dissertation, plasma treatment, chemical doping and functionalization methods have been applied to tune the properties of TMDCs. First, plasma treatment of TMDCs results in doping and generation of defects, as well as the synthesis of transition metal oxides (TMOs) with rolled layers that have increased surface-to-volume ratio and are promising for electrochemical applications. Second, chemical functionalization is another powerful approach for tuning the properties of TMDCs for use in many applications. To covalently functionalize the basal planes of TMDCs, previous reports begin with harsh treatments like lithium intercalation that disrupt the structure and lead to a phase transformation from semiconducting to metallic. Instead, this work demonstrates the direct covalent functionalization of semiconducting MoS2 using aryl diazonium salts without lithium treatments. It preserves the structure and semiconducting nature of MoS2, results in covalent C-S bonds on basal planes and enables different functional groups to be tethered to the MoS2 surface via the diazonium salts. The attachment of fluorescent proteins has been used as a demonstration and it suggests future applications in biology and biosensing. The effects of the covalent functionalization on the electronic transport properties of MoS2 were then studied using field effect transistor (FET) devices.
ContributorsChu, Ximo (Author) / Wang, Qing Hua (Thesis advisor) / Sieradzki, Karl (Committee member) / Green, Alexander (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2018
Fill Factor Loss Mechanisms: Analysis and Basic Understanding in Silicon Hetero-junction Solar Cells
Description
The objective of this thesis is to achieve a detailed understanding of the loss mechanisms in SHJ solar cells. The working principles of these cells and what affects the cell operation, e.g. the IV characteristics at the maximum power point (MPP) and the correspondingly ll factor (FF) are investigated. Dierent loss sources are analyzed separately, and the weight of each in the total loss at the MPP are evaluated. The total series resistance is measured and then compared with the value obtained through summation over each of its components. In other words, series resistance losses due to recombination, vertical and lateral carrier transport, metalization, etc, are individually evaluated, and then by adding all these components together, the total loss is calculated. The concept of ll factor and its direct dependence on the loss mechanisms at the MPP of the device is explained, and its sensitivity to nearly every processing step of the cell fabrication is investigated. This analysis provides a focus lens to identify the main source of losses in SHJ solar cells and pave the path for further improvements in cell efficiency.
In this thesis, we provide a detailed understanding of the FF concept; we explain how it can be directly measured; how it can be calculated and what expressions can better approximate its value and under what operating conditions. The relation between FF and cell operating condition at the MPP is investigated. We separately analyzed the main FF sources of losses including recombination, sheet resistance, contact resistance and metalization. We study FF loss due to recombination and its separate components which include the Augur, radiative and SRH recombination is investigated. We study FF loss due to contact resistance and its separate components which include the contact resistance of dierent interfaces, e.g. between the intrinsic and doped a-Si layers, TCO and a-Si layers. We also study FF loss due to lateral transport and its components that including the TCO sheet resistance, the nger and the busbars resistances.
In this thesis, we provide a detailed understanding of the FF concept; we explain how it can be directly measured; how it can be calculated and what expressions can better approximate its value and under what operating conditions. The relation between FF and cell operating condition at the MPP is investigated. We separately analyzed the main FF sources of losses including recombination, sheet resistance, contact resistance and metalization. We study FF loss due to recombination and its separate components which include the Augur, radiative and SRH recombination is investigated. We study FF loss due to contact resistance and its separate components which include the contact resistance of dierent interfaces, e.g. between the intrinsic and doped a-Si layers, TCO and a-Si layers. We also study FF loss due to lateral transport and its components that including the TCO sheet resistance, the nger and the busbars resistances.
ContributorsLeilaeioun, Mohammadmehdi (Ashling) (Author) / Goodnick, Stephen (Thesis advisor) / Goryll, Michael (Thesis advisor) / Bertoni, Mariana (Committee member) / Bowden, Stuart (Committee member) / Stuckelberger, Michael (Committee member) / Arizona State University (Publisher)
Created2018
Description
There has been a surge in two-dimensional (2D) materials field since the discovery of graphene in 2004. Recently, a new class of layered atomically thin materials that exhibit in-plane structural anisotropy, such as black phosphorous, transition metal trichalcogenides and rhenium dichalcogenides (ReS2), have attracted great attention. The reduced symmetry in these novel 2D materials gives rise to highly anisotropic physical properties that enable unique applications in next-gen electronics and optoelectronics. For example, higher carrier mobility along one preferential crystal direction for anisotropic field effect transistors and anisotropic photon absorption for polarization-sensitive photodetectors.
This dissertation endeavors to address two key challenges towards practical application of anisotropic materials. One is the scalable production of high quality 2D anisotropic thin films, and the other is the controllability over anisotropy present in synthesized crystals. The investigation is focused primarily on rhenium disulfide because of its chemical similarity to conventional 2D transition metal dichalcogenides and yet anisotropic nature. Carefully designed vapor phase deposition has been demonstrated effective for batch synthesis of high quality ReS2 monolayer. Heteroepitaxial growth proves to be a feasible route for controlling anisotropic directions. Scanning/transmission electron microscopy and angle-resolved Raman spectroscopy have been extensively applied to reveal the structure-property relationship in synthesized 2D anisotropic layers and their heterostructures.
This dissertation endeavors to address two key challenges towards practical application of anisotropic materials. One is the scalable production of high quality 2D anisotropic thin films, and the other is the controllability over anisotropy present in synthesized crystals. The investigation is focused primarily on rhenium disulfide because of its chemical similarity to conventional 2D transition metal dichalcogenides and yet anisotropic nature. Carefully designed vapor phase deposition has been demonstrated effective for batch synthesis of high quality ReS2 monolayer. Heteroepitaxial growth proves to be a feasible route for controlling anisotropic directions. Scanning/transmission electron microscopy and angle-resolved Raman spectroscopy have been extensively applied to reveal the structure-property relationship in synthesized 2D anisotropic layers and their heterostructures.
ContributorsChen, Bin, 1968- (Author) / Tongay, Sefaattin (Thesis advisor) / Bertoni, Mariana (Committee member) / Chang, Lan-Yun (Committee member) / Arizona State University (Publisher)
Created2018
Description
Achieving high efficiency in solar cells requires optimal photovoltaics materials for light absorption and as with any electrical device—high-quality contacts. Essentially, the contacts separate the charge carriers—holes at one terminal and electrons at the other—extracting them to an external circuit. For this purpose, the development of passivating and carrier-selective contacts that enable low interface defect density and efficient carrier transport is critical for making high-efficiency solar cells. The recent record-efficiency n-type silicon cells with hydrogenated amorphous silicon (a-Si:H) contacts have demonstrated the usefulness of passivating and carrier-selective contacts. However, the use of a-Si:H contacts should not be limited in just n-type silicon cells.
In the present work, a-Si:H contacts for crystalline silicon and cadmium telluride (CdTe) solar cells are developed. First, hydrogen-plasma-processsed a-Si:H contacts are used in n-type Czochralski silicon cell fabrication. Hydrogen plasma treatment is used to increase the Si-H bond density of a-Si:H films and decrease the dangling bond density at the interface, which leads to better interface passivation and device performance, and wider temperature-processing window of n-type silicon cells under full spectrum (300–1200 nm) illumination. In addition, thickness-varied a-Si:H contacts are studied for n-type silicon cells under the infrared spectrum (700–1200 nm) illumination, which are prepared for silicon-based tandem applications.
Second, the a-Si:H contacts are applied to commercial-grade p-type silicon cells, which have much lower bulk carrier lifetimes than the n-type silicon cells. The approach is using gettering and bulk hydrogenation to improve the p-type silicon bulk quality, and then applying a-Si:H contacts to enable excellent surface passivation and carrier transport. This leads to an open-circuit voltage of 707 mV in p-type Czochralski silicon cells, and of 702 mV, the world-record open-circuit voltage in p-type multi-crystalline silicon cells.
Finally, CdTe cells with p-type a-Si:H hole-selective contacts are studied. As a proof of concept, p-type a-Si:H contacts enable achieving the highest reported open-circuit voltages (1.1 V) in mono-crystalline CdTe devices. A comparative study of applying p-type a-Si:H contacts in poly-crystalline CdTe solar cells is performed, resulting in absolute voltage gain of 53 mV over using the standard tellurium contacts.
In the present work, a-Si:H contacts for crystalline silicon and cadmium telluride (CdTe) solar cells are developed. First, hydrogen-plasma-processsed a-Si:H contacts are used in n-type Czochralski silicon cell fabrication. Hydrogen plasma treatment is used to increase the Si-H bond density of a-Si:H films and decrease the dangling bond density at the interface, which leads to better interface passivation and device performance, and wider temperature-processing window of n-type silicon cells under full spectrum (300–1200 nm) illumination. In addition, thickness-varied a-Si:H contacts are studied for n-type silicon cells under the infrared spectrum (700–1200 nm) illumination, which are prepared for silicon-based tandem applications.
Second, the a-Si:H contacts are applied to commercial-grade p-type silicon cells, which have much lower bulk carrier lifetimes than the n-type silicon cells. The approach is using gettering and bulk hydrogenation to improve the p-type silicon bulk quality, and then applying a-Si:H contacts to enable excellent surface passivation and carrier transport. This leads to an open-circuit voltage of 707 mV in p-type Czochralski silicon cells, and of 702 mV, the world-record open-circuit voltage in p-type multi-crystalline silicon cells.
Finally, CdTe cells with p-type a-Si:H hole-selective contacts are studied. As a proof of concept, p-type a-Si:H contacts enable achieving the highest reported open-circuit voltages (1.1 V) in mono-crystalline CdTe devices. A comparative study of applying p-type a-Si:H contacts in poly-crystalline CdTe solar cells is performed, resulting in absolute voltage gain of 53 mV over using the standard tellurium contacts.
ContributorsShi, Jianwei (Author) / Holman, Zachary (Thesis advisor) / Bowden, Stuart (Committee member) / Bertoni, Mariana (Committee member) / Goodnick, Stephen (Committee member) / Arizona State University (Publisher)
Created2018
Description
In this dissertation, micro-galvanic corrosion effects and passivation behavior of single-phase binary alloys have been studied in order to formulate new insights towards the development of “stainless-like” lightweight alloys. As a lightweight material of interest, Mg-xAl alloys were studied using aqueous free corrosion, atmospheric corrosion, dissolution rate kinetics, and ionic liquid dissolution. Polarization and “accelerated” free corrosion studies in aqueous chloride were used to characterize the corrosion behavior and morphology of alloys. Atmospheric corrosion experiments revealed surface roughness and pH evolution behavior in aqueous environment. Dissolution in absence of water using choline-chloride:urea ionic liquid allowed for a simpler dissolution mechanism to be observed, providing additional insights regarding surface mobility of Al. These results were compared with commercial alloy (AZ31B, AM60, and AZ91D) behavior to better elucidate effects associated with secondary phases and intermetallic particles often present in Mg alloys. Aqueous free corrosion, “accelerated” free corrosion and ionic liquid dissolution studies have confirmed Al surface enrichment in a variety of morphologies, including Al-rich platelet and Al nanowire formation. This behavior is attributed to the preferential dissolution of Al as the more “noble” element in the matrix. Inductively-coupled mass spectroscopy was used to measure first-order rate reaction constants for elemental Mg and Al dissolution in aqueous chloride environment to be kMg= 9.419 x 10-6 and kAl = 2.103 x 10-6 for future implementation in kinetic Monte Carlo simulations. To better understand how “stainless-like” passivation may be achieved, Ni-xCr alloys were studied using polarization and potential pulse experiments. The passivation potential, critical current density, and passivation current density were found to decay with increasing Cr composition. The measured average number of monolayers dissolved during passivation was found to be in good agreement with percolation theory, with a fitted 3-D percolation threshold of p_c^3D=0.118 compared with the theoretical value of 0.137. Using these results, possible approaches towards achieving passivation in other systems, including Mg-Al, are discussed.
ContributorsAiello, Ashlee (Author) / Sieradzki, Karl (Thesis advisor) / Buttry, Daniel (Committee member) / Chan, Candace (Committee member) / Crozier, Peter (Committee member) / Arizona State University (Publisher)
Created2018
Description
With the world's ever growing need for sustainable energy solutions, the field of thermoelectrics has seen rejuvenated interest. Specifically, modern advances in nanoscale technology have resulted in predictions that thermoelectric devices will soon become a viable waste heat recovery energy source, among other things. In order to achieve these predictions, however, key structure-property relationships must first be understood. Currently, the Thermal Energy and Nanomaterials Lab at Arizona State University is attempting to solve this problem. This project intends to aid the groups big picture goal by developing a robust and user friendly measurement platform which is capable of reporting charge carrier mobility, electrical conductivity, and Seebeck coefficient values. To date, the charge carrier mobility and electrical conductivity measurements have been successfully implemented and validated. First round analysis has been performed on β-In2Se3 thin film samples. Future work will feature a more comprehensive analysis of this material.
ContributorsNess, Kyle David (Author) / Wang, Robert (Thesis director) / Chan, Candace (Committee member) / Barrett, The Honors College (Contributor) / Mechanical and Aerospace Engineering Program (Contributor)
Created2014-05