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Title: Investigation on the Mechanical, Microstructural, and Electrical Properties of Graphene Oxide-Cement Composite.
Creator: Al Muhit, Baig Abdullah, Nam, Boo Hyun, Zhai, Lei, Chopra, Manoj, University of Central Florida
Abstract / Description: Nanotechnology refers to the use of the materials or particles ranging from a few nanometers (nm) to 100 nanometers (nm) in a wide range of applications. Use of nanomaterials in cement composite to enhance the mechanical properties, fracture toughness and other functionalities has been studied for decades. In this regard, one of the carbon-based nanomaterials, Graphene Oxide (GO), has received attentions from researchers for its superior mechanical properties (e.g. tensile strength, yield...
Show moreNanotechnology refers to the use of the materials or particles ranging from a few nanometers (nm) to 100 nanometers (nm) in a wide range of applications. Use of nanomaterials in cement composite to enhance the mechanical properties, fracture toughness and other functionalities has been studied for decades. In this regard, one of the carbon-based nanomaterials, Graphene Oxide (GO), has received attentions from researchers for its superior mechanical properties (e.g. tensile strength, yield strength, and Young's modulus). Although GO is not lucrative in increasing electrical conductivity (EC) of cement paste compared to that of graphene- another derivative of GO, reduced graphene oxide (rGO), might be a solution to increase EC. Another derivative of GO is the solution to the problem.In this research, the compressive strength and flexural strength of GO-cement composite (GOCC) and rGO-cement composite (rGOCC) have been investigated with 0.01% and 0.05% GO and rGO content. GOCC-0.05% showed 27% increase in compressive strength compared to the control cement paste after 28 days (d) of hydration. GOCC-0.01% showed only 3.4% increase in compressive strength compared to the control. rGOCC-0.05% showed 21% increase in compressive strength and 15.5% increase in Modulus of Rupture (MOR) compared to the control cement paste after 28 d of hydration. On the other hand, rGOCC-0.01% showed 7% increase in compressive strength and 0.35% increase in MOR after 28 d. GOCC-0.05% showed increasing trends in compressive strength after 28 d indicating continuation of hydration. Similarly, rGOCC-0.05% also showed increasing trends in compressive and flexural strength after 28 d, possibly due to the reason described earlier.Microstructural investigation on GOCC-0.05% and GOCC-0.01% by X-ray Diffraction (XRD) illustrated that the crystallite sizes of tobermorite-9(&)#197; and jennite, which are mineralogical counterpart of disordered Calcium-Silicate-Hydrate (C-S-H), increases from 3 d to 28 d, representing the crystallite growth due to continued hydration. However, the crystallite size of GOCC-0.05% was smaller than that of GOCC-0.01% at both 3 d and 28 d, indicating finer nucleated grains. According to Hall-Petch equation, mechanical strength increases with decreasing particle size. Finer particles or grains can increase the strength in cement composites in several other ways: (1) GO acted as heterogeneous nucleation sites because of reactive functional groups. Activation energy was decreased by these (")defects(") in the cement paste, and consequently, numerous nuclei of C-S-H. with high surface area were formed, (2) because of finer grains, cracks are forced to move along a tortuous path, which makes the structure difficult to fail, and strength increased consequently (3) Finer grains of GOCC-0.05% created compacted hydration products decreasing porosity which can indirectly increase the strength. The above reasons, separately or in conjunction, might increase the strength of GOCC-0.05% and proved that GO is responsible for increasing heterogeneous nucleation sites during cement hydration.Early age hydration (EAH) characteristics were investigated for rGOCC specimens with 0.1% and 0.5% rGO content. Scanning Electron Microscope (SEM), Energy Dispersive X-ray analysis (EDX), and X-ray Diffraction (XRD) were employed to study the EAH characteristics. SEM/EDX, and XRD analysis were performed after 15 min, 1 h, 3 h and 24 h of hydration. (EAH) study on rGOCC-0.1% showed that at 15 m(&)#172;in hydration, numerous precipitates of, possibly, C-S-H formed along the grain boundary (GB) of unhydrated cement grains. This served as visual confirmation of Thomas and Scherer's Boundary Nucleation and Growth (BNG) model that hydration of cement grains was initiated by the short burst of nucleation of C-S-H embryos along GB. EDX on rGOCC-0.1% and rGOCC-0.5% showed that Ca/Si ratio in C-S-H was ~2.0. This finding indicated that C-S-H structure in this study was concurrent with that of impure jennite. XRD analysis also evidently showed that jennite was present, possibly possessing a short range ordered (SRO) structure, referring to local crystalline structure in a very short area. After consulting Chen's work, it would be appropriate to say that C-S-H found in this study resembled more as C-S-H (II), which is disordered jennite. It was also observed that as expected with cement with nanomaterials, with continuing hydration, pore spaces were filled with hydration products such as C-S-H, ettringite, CH, sulfoaluminates etc,.Lastly, Electrical resistivity (ER) testing on 9 sets of rGOCC specimens was conducted. The specimen includes 0.5%, 1%, 5% rGO content, and the control conditioned in both oven dry (OD) and saturated surface dry (SSD). ER increased with the increase of rGO content from 0.5% and 1% compared to that of the control. However, the ER of rGOCC-5% was significantly decreased, showing 93% reduction compared to the control, which can be interpreted as a threshold value for sensing applications to be explored. As expected, large reduction of ER value occurred on the specimens with the SSD condition. This reduction can be attributed to the ionic conduction though the pore solution of the composites. As the rGO content increased, so did the potential nucleation sites for hydration (as can be seen in SEM images), which might block the number of contact points among the rGO, resulting in low conduction and high resistivity. However, as rGO content increased to 5%, the contact areas/points increased to a degree that could trump the nucleation seeding sites, resulting in decreased ER. The ER measured with the rGOCC specimens was comparable to that of cement composites incorporating carbon fibers (CF), and steel fibers, but higher content of rGO are required to have a similar ER range of those fiber cement composites. This might be due to smaller sizes of rGO sheets and lower aspect ratio compared to other nanofibers causing drastic reduction of electron tunneling mechanism compared to other fibers.
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Date Issued: 2015
Identifier: CFE0005752, ucf:50107
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005752

Title: Real time monitoring of Cell-Nanoparticles interaction and tracking internalization process by mechanical probing using Atomic Force Microscopy.
Creator: Ly, Anh, Seal, Sudipta, Zhai, Lei, Heinrich, Helge, University of Central Florida
Abstract / Description: With extensive development of nanotechnology in last few years, scientists have discovered that nanoparticles (NPs) can be used as an efficient Drug Delivery System (DOS). In order to develop better NPs based drug delivery tool, it is imperative to understand the interaction between the NPs and the cell membrane. In our earlier studies, cerium oxide nanoparticles (CNPs) have been reported to have therapeutic properties, specifically against abnormalities associated with oxidative stress....
Show moreWith extensive development of nanotechnology in last few years, scientists have discovered that nanoparticles (NPs) can be used as an efficient Drug Delivery System (DOS). In order to develop better NPs based drug delivery tool, it is imperative to understand the interaction between the NPs and the cell membrane. In our earlier studies, cerium oxide nanoparticles (CNPs) have been reported to have therapeutic properties, specifically against abnormalities associated with oxidative stress. Therefore, CNPs with different sizes and morphology were selected to understand the interaction with cell. We analyzed the mechanical property of human nasal septum tumor cells membranes using Atomic Force Microscopy (AFM) with and without CNPs. In particular, Force-Distance spectroscopy mode was used to estimate the elasticity of cells membrane. Different concentrations (0, 50, 125 and 250 ?M) of CNPs were added to the cells (squamous cells; CCL30) and incubated for different time periods (0, 15, 30 and 60 minutes). Cell membrane elasticity/Young's modulus was calculated using a modified Hertz model. Changes in the cell elasticity were observed in high concentration of CNPs when treated with one hour. Significant changes in cell elasticity were observed at high concentration of CNPs for one hour of incubation. No significant change in cell elasticity was observed over one hour time period for 50 ?M of CNPs. Moreover, by using selected inhibitors to block different cell mediated internalization pathways, we also investigated the correlation between the cellular uptake and the tracking of NPs with their size. Specifically, similar change in cell elasticity was observed after blocking the cell energy production for CNPs with smaller diameter (3-5 nm). On the other hand, bigger size NPs (20-30 nm) showed no change in cell elasticity after blocking the cell energy production. These results indicate that 3-5 nm particles internalize cell by non-energy dependent pathway i.e. passive diffusion whereas 20-30 nm particles entered in cell by energy dependent pathways i.e. endocytosis of particles. Further, we have also identified the cellular uptake of 20-30 nm particles is by enclosing those CNPs in membrane vesicles in caveolae-mediated endocytosis mechanism. In summary, these results indicate that the nanoparticles-cell interaction has pronounced influence on the shape and size of the nanoparticles. These interactions can be further monitored by real time mechanical property measurement of cell membrane.
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Date Issued: 2014
Identifier: CFE0005204, ucf:50637
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005204

Title: Graphene Induced Formation of Nanostructures in Composites.
Creator: Shen, Chen, Zhai, Lei, Chen, Quanfang, Thomas, Jayan, Fang, Jiyu, Khondaker, Saiful, University of Central Florida
Abstract / Description: Graphene induced nanostructures in graphene-based composites and the performance of these composites have been explored in this study. For the metallic nanoparticles decorated graphene aerogels composites, the fabrication of hierarchically structured, reduced graphene oxide (rGO) aerogels with heavily metallic nanoparticles was realized. Higher loading of palladium nanoparticles in graphene aerogels leads to improved hydrogen gas sensing performance. For polymer derived ceramics (PDCs)...
Show moreGraphene induced nanostructures in graphene-based composites and the performance of these composites have been explored in this study. For the metallic nanoparticles decorated graphene aerogels composites, the fabrication of hierarchically structured, reduced graphene oxide (rGO) aerogels with heavily metallic nanoparticles was realized. Higher loading of palladium nanoparticles in graphene aerogels leads to improved hydrogen gas sensing performance. For polymer derived ceramics (PDCs) composites with anisotropic electrical properties, the fabrication of composites was realized by embedding anisotropic reduced graphene oxide aerogels (rGOAs) into the PDCs matrix. Raman spectroscopy and X-ray diffraction studies of PDCs composites with and without graphene indicate that graphene facilitates the transition from amorphous carbon to graphitic carbon in the PDCs. For composites composed of PDCs and edge functionalized graphene oxide (EFGO), bulk PDCs based composites with embedded graphene networks show high electrical conductivity, high thermal stability, and low thermal conductivity. For the study of poly(3-hexylthiophene) (P3HT) crystallization on graphitic substrates (i.e. carbon nanotubes, carbon fibers and graphene), different types of P3HT nanocrystals (i.e. nanowires, nanoribbons, and nanowalls) were observed. The type of nanocrystals grown from graphitic substrates depends on the curvature of graphitic substrates, the molecular weight of P3HT molecules, and the concentration of P3HT marginal solutions. Besides, both specific surface area and curvature of graphitic substrates have major effects on P3HT crystallization processes.
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Date Issued: 2018
Identifier: CFE0007095, ucf:51961
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007095

Title: Nanoplasmonics In Two-dimensional Dirac and Three-dimensional Metallic Nanostructure Systems.
Creator: Safaei, Alireza, Chanda, Debashis, Leuenberger, Michael, Mucciolo, Eduardo, Tetard, Laurene, Zhai, Lei, University of Central Florida
Abstract / Description: Surface plasmons are collective oscillation of electrons which are coupled to the incident electric field. Excitation of surface plasmon is a route to engineer the behavior of light in nanometer length scale and amplifying the light-matter interaction. This interaction is an outcome of near-field enhancement close to the metal surface which leads to plasmon damping through radiative decay to outgoing photons and nonradiative decay inside and on the surface of the material to create an...
Show moreSurface plasmons are collective oscillation of electrons which are coupled to the incident electric field. Excitation of surface plasmon is a route to engineer the behavior of light in nanometer length scale and amplifying the light-matter interaction. This interaction is an outcome of near-field enhancement close to the metal surface which leads to plasmon damping through radiative decay to outgoing photons and nonradiative decay inside and on the surface of the material to create an electron-hole pair via interband or intraband Landau damping. Plasmonics in Dirac systems such as graphene show novel features due to massless electrons and holes around the Dirac cones. Linear band structure of Dirac materials in the low-momentum limit gives rise to the unprecedented optical and electrical properties. Electronical tunability of the plasmon resonance frequency through applying a gate voltage, highly confined electric field, and low plasmon damping are the other special propoerties of the Dirac plasmons. In this work, I will summarize the theoretical and experimental aspects of the electrostatical tunable systems made from monolayer graphene working in mid-infrared regime. I will demonstrate how a cavity-coupled nanopatterned graphene excites Dirac plasmons and enhances the light-matter interaction. The resonance frequency of the Dirac plasmons is tunable by applying a gate voltage. I will show how different gate-dielectrics, and the external conditions like the polarization and angle of incident light affect on the optical response of the nanostructure systems. I will then show the application of these nanodevices in infrared detection at room temperature by using plasmon-assisted hot carriers generation. An asymmetric nanopatterned graphene shows a high responsivity at room temperature which is unprecedented. At the end, I will demonstrate the properties of surface plasmons on 3D noble metals and its applications in light-funneling, photodetection, and light-focusing.
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Date Issued: 2019
Identifier: CFE0007904, ucf:52746
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007904

Title: Light Scattering Property of Gold Nanoparticles with Applications to Biomolecule Detection and Analysis.
Creator: Zheng, Tianyu, Huo, Qun, Zou, Shengli, Gesquiere, Andre, Kang, Hyeran, Zhai, Lei, University of Central Florida
Abstract / Description: Gold nanoparticles (AuNPs) have unique optical and chemical properties. Dynamic light scattering (DLS) is an analytical tool used routinely for nanoparticle size measurement. The combined use of AuNPs and DLS has led to a novel analytical assay technology called D2Dx (from diameter to diagnostics). Herein, my dissertation highlights the extended use of D2Dx for biomolecule detection and analysis. Under this general theme, Chapter 1 provides some background information of AuNPs, DLS, the...
Show moreGold nanoparticles (AuNPs) have unique optical and chemical properties. Dynamic light scattering (DLS) is an analytical tool used routinely for nanoparticle size measurement. The combined use of AuNPs and DLS has led to a novel analytical assay technology called D2Dx (from diameter to diagnostics). Herein, my dissertation highlights the extended use of D2Dx for biomolecule detection and analysis. Under this general theme, Chapter 1 provides some background information of AuNPs, DLS, the principle of D2Dx technique and its potential applications. Chapter 2 summarizes a study on the effect of AuNP concentrations and laser power on the hydrodynamic size measurement of AuNPs by DLS. This study demonstrated the multiple scattering effect on DLS analysis, and how to use the exceptionally high sensitivity of DLS in AuNP aggregate detection for bioassay design and development. Chapter 3 explores a cooperative interaction between AuNP and certain proteins in blood serum that are key to the immune system, leading to a novel diagnostic tool that can conveniently monitor the humoral immunity development from neonates to adults and detect active infections in animals. Chapter 4 reports an application of D2Dx technique for acute viral infection detection based on the active immune responses elicited from mouse models infected with influenza virus. Chapter 5 describes another application of D2Dx for prostate cancer detection. The D2Dx assay identifies prostate cancer patients from non-cancer controls with improved specificity and sensitivity than PSA test. Chapter 6 demonstrates the use of AuNPs and DLS for hydrodynamic size measurement of protein disulfide isomerase with two different conformations. Chapter 7 investigates the concentration-dependent self-assembling behavior of ribostamycin through its interaction with AuNPs in aqueous solution. Overall, this dissertation established several lines of applications of using AuNPs and DLS for biomolecular research and in vitro diagnostics.
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Date Issued: 2018
Identifier: CFE0007385, ucf:52056
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007385

Title: Polyelectrolyte complexes based on poly(acrylic acid): mechanics and applications.
Creator: Lu, Xiaoyan, Zhai, Lei, Zou, Shengli, Chumbimuni Torres, Karin, Kolpashchikov, Dmitry, Dong, Yajie, University of Central Florida
Abstract / Description: Poly(acrylic acid) (PAA) is a weak polyelectrolyte presenting negative charge at basic conditionwhen the carboxylic group loses a proton. These carboxylate group can interact with polycationsand metal ions to form stable polyelectrolyte complexes (PECs), leading to tunable propertiesand multifunctional nanoscale structures through chemical reactions. This research focuses onnanofiber and nanoparticle fabricated by PAA-based PECs. We demonstrated the effect of ferricion concentration on the...
Show morePoly(acrylic acid) (PAA) is a weak polyelectrolyte presenting negative charge at basic conditionwhen the carboxylic group loses a proton. These carboxylate group can interact with polycationsand metal ions to form stable polyelectrolyte complexes (PECs), leading to tunable propertiesand multifunctional nanoscale structures through chemical reactions. This research focuses onnanofiber and nanoparticle fabricated by PAA-based PECs. We demonstrated the effect of ferricion concentration on the mechanical properties of PAA-based single naonofiber by using dark fieldmicroscopy imaging and persistence length analysis. The application of PAA-based nanofibermats loaded with MnO2 for supercapacitors was also explored. As a free-standing and flexiblesupercapacitor electrode, the nanofiber mat exhibited outstanding properties including high specificcapacitance, excellent reversible redox reactions, and fast charge/discharge ability. Since PAA is abiocompatible polymer, PAA-based PEC was applied as a drug-carrier in a drug delivery system.In this project, core-shell nanoparticles were fabricated with chitosan as the core and PAA as theshell to incorporate with the drug gemcitabine. Several parameters were investigated to obtainthe optimal nanoparticle size. The as-prepared drug delivery system shows prolonged releasingprofile.
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Date Issued: 2018
Identifier: CFE0007045, ucf:52004
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007045

Title: Optical Properties of Single Nanoparticles and Two-dimensional Arrays of Plasmonic Nanostructures.
Creator: Zhou, Yadong, Zou, Shengli, Harper, James, Zhai, Lei, Chen, Gang, Zheng, Qipeng, University of Central Florida
Abstract / Description: The tunability of plasmonic properties of nanomaterials makes them promising in many applications such as molecular detection, spectroscopy techniques, solar energy materials, etc. In the thesis, we mainly focus on the interaction between light with single nanoparticles and two-dimensional plasmonic nanostructures using electrodynamic methods. The fundamental equations of electromagnetic theory: Maxwell's equations are revisited to solve the problems of light-matter interaction, particularly...
Show moreThe tunability of plasmonic properties of nanomaterials makes them promising in many applications such as molecular detection, spectroscopy techniques, solar energy materials, etc. In the thesis, we mainly focus on the interaction between light with single nanoparticles and two-dimensional plasmonic nanostructures using electrodynamic methods. The fundamental equations of electromagnetic theory: Maxwell's equations are revisited to solve the problems of light-matter interaction, particularly the interaction of light and noble nanomaterials, such as gold and silver. In Chapter 1, Stokes parameters that describe the polarization states of electromagnetic wave are presented. The scattering and absorption of a particle with an arbitrary shape are discussed. In Chapter 2, several computational methods for solving the optical response of nanomaterials when they are illuminated by incident light are studied, which include the Discrete Dipole Approximation (DDA) method, the coupled dipole (CD) method, etc. In Chapter 3, the failure and reexamination of the relation between the Raman enhancement factor and local enhanced electric field intensity is investigated by placing a molecular dipole in the vicinity of a silver rod. Using a silver rod and a molecular dipole, we demonstrate that the relation generated using a spherical nanoparticle cannot simply be applied to systems with particles of different shapes. In Chapter 4, a silver film with switchable total transmission/reflection is discussed. The film is composed of two-dimensional rectangular prisms. The factors affecting the transmission (reflection) as well as the mechanisms leading to the phenomena are studied. Later, in Chapter 5 and 6, the sandwiched nano-film composed of two 2D rectangular prisms arrays and two glass substrates with a continuous film in between is examined to enhance the transmission of the continuous silver film.
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Date Issued: 2018
Identifier: CFE0007117, ucf:51943
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007117

Title: nanoengineered energy harvesting and storage devices.
Creator: Li, Chao, Thomas, Jayan, Zhai, Lei, Yang, Yang, Gesquiere, Andre, Dong, Yajie, Sun, Wei, University of Central Florida
Abstract / Description: Organic and perovskite solar cells have recently attracted significant attention due to itsflexibility, ease of fabrication and excellent performance. In order to realize even betterperformance for organic and perovskite solar cells, rejuvenated effort towards developingnanostructured electrodes and high quality active layer is necessary.In this dissertation, several strategic directions of enhancing the performance of organicand perovskite solar cells are investigated. An introduction and...
Show moreOrganic and perovskite solar cells have recently attracted significant attention due to itsflexibility, ease of fabrication and excellent performance. In order to realize even betterperformance for organic and perovskite solar cells, rejuvenated effort towards developingnanostructured electrodes and high quality active layer is necessary.In this dissertation, several strategic directions of enhancing the performance of organicand perovskite solar cells are investigated. An introduction and background of organic andperovskite solar cells, which includes motivation, classification and working principles,nanostructured electrode materials and solvent effect on active materials, and devices fabrication,are presented. A facile method, called Spin-on Nanoprinting (SNAP), to fabricate highly orderedZnO-AgNW-ZnO electrode is introduced to enhance the performance of organic solar cell.Subsequently, a ternary solvent method is developed to fabricate high Voc thieno[3,4-b]thiophene/benzodithiophene (PTB7) and indene-C60 bisadduct (ICBA)solar cells. Theperformance of the devices improved about 20% compared to those made by binary solventmethod. In order to understand the fundamental properties of the materials ruling theperformance of the PSCs tested, AFM-based nanoscale characterization techniques includingPulsed-Force-Mode AFM (PFM-AFM) and Mode-Synthesizing AFM (MSAFM) are introduced.These methods are used to study the morphology and physical properties of the structuresconstitutive of the active layers of the PSCs. Conductive-AFM (cAFM) studies reveal localvariations in conductivity in the donor and acceptor phases as well as an increase in photocurrentmeasured in the PTB7:ICBA sample obtained with the ternary solvent processing technique.Moreover, efficient perovskite solar cells with good transparency in the visible wavelength rangehave been developed by a facile and low-temperature PCBM-assisted perovskite growth method.This method results in the formation of perovskite-PCBM hybrid material at the grain boundaries which is observed by EELS mapping and confirmed by steady-state photoluminescence (PL)spectra and transient photocurrent (TP) measurements. This method involves fewer steps andtherefore is less expensive and time consuming than other reported methods. In addition, wereport an all solid state, energy harvesting and storing (ENHANS) filament which integratesperovskite solar cell (PSC) on top of a symmetric supercapacitor (SSC) via a copper filamentwhich works as a shared electrode for direct charge transfer. Developing ENHANS on a copperfilament provides a low-cost solution for flexible self-sufficient energy systems for wearablesand other portable devices. Finally, a summary of this dissertation as well as some potentialfuture directions are presented.
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Date Issued: 2016
Identifier: CFE0006693, ucf:51912
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0006693

Title: Regolith-Based Construction Materials for Lunar and Martian Colonies.
Creator: Grossman, Kevin, Seal, Sudipta, Florczyk, Stephen, Fang, Jiyu, Zhai, Lei, Leuenberger, Michael, University of Central Florida
Abstract / Description: Humankind's ambitions of exploring our solar system and parts beyond depend heavily on our ability to collect resources from local environments at our destinations rather than bringing materials on the journey. This is a concept known as in-situ resource utilization (ISRU) and it is one that has been understood by every explorer and settler in the history of humankind. Regolith on the moon and Mars has been shown to be a particularly useful resource and has the ability to provide humans with...
Show moreHumankind's ambitions of exploring our solar system and parts beyond depend heavily on our ability to collect resources from local environments at our destinations rather than bringing materials on the journey. This is a concept known as in-situ resource utilization (ISRU) and it is one that has been understood by every explorer and settler in the history of humankind. Regolith on the moon and Mars has been shown to be a particularly useful resource and has the ability to provide humans with resources including water, oxygen, construction material, fabric, radiation shielding, metals, and may more. This dissertation focuses on construction materials derived from standard regolith simulant JSC-1A, including bricks, composites, metals and modified powder materials. Sintering processes with JSC-1A were studied to determine optimal heating profiles and resulting compressive strengths. It was determined that the temperature profiles have an optimal effect on smaller particle sizes due to the larger surface area to volume ratio of small particles and sintering being a surface event. Compressive strengths of sintered regolith samples were found to be as high as 38,000 psi, which offers large utility for martian or lunar colonies. This study also investigates a method for extracting metals from regolith known as molten regolith electrolysis. The alloy of the two major metallic components of regolith, iron and silicon, has been investigated as a structural metal for colonies and a potential feedstock for novel metallic 3D printers. Parallel to these efforts, a new additive manufacturing technique designed to print metal parts in low and zero gravity environments is developed. The mechanical properties from metal parts from this technique are examined and it is determined how the printing process determines a microstructure within the steel that impacts the utility of the technology.
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Date Issued: 2018
Identifier: CFE0007331, ucf:52144
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007331

Title: INTERFACIAL BEHAVIOR IN POLYMER DERIVED CERAMICS AND SALT WATER PURIFICATION VIA 2D MOS2.
Creator: Li, Hao, An, Linan, Jung, YeonWoong, Zhai, Lei, Feng, Xiaofeng, Yu, Xiaoming, University of Central Florida
Abstract / Description: In the present dissertation, the behavior of the internal potential barrier in a polymer-derived amorphous SiAlCN ceramic was studied by measuring its complex impedance spectra at various dc bias as well as different testing and annealing temperatures. The complex impedancespectra of the polymer-derived a-SiAlCN were measured under various dc bias voltages in a temperature range between 50 and 150?(&)deg;C, as well as different annealing temperatures (1100-1400 (&)deg;C). All spectra,...
Show moreIn the present dissertation, the behavior of the internal potential barrier in a polymer-derived amorphous SiAlCN ceramic was studied by measuring its complex impedance spectra at various dc bias as well as different testing and annealing temperatures. The complex impedancespectra of the polymer-derived a-SiAlCN were measured under various dc bias voltages in a temperature range between 50 and 150?(&)deg;C, as well as different annealing temperatures (1100-1400 (&)deg;C). All spectra, regardless of temperature and bias, consist of two semi-circular arcs,corresponding to the free-carbon phase and the interface, respectively. The impedance of the free-carbon phase is independent of the bias, while that of the interface decreased significantly with increasing dc bias. It is shown that the change of the interfacial capacitance with the bias can be explained using the double Schottky barrier model. The charge-carrier concentration and potential barrier height were estimated by comparing the experimental data and the model.The results revealed that increasing testing temperature led to an increased charge-carrier concentration and a reduced barrier height, both following Arrhenius dependence, whereas the increase in annealing temperature resulted in increased charge-carrier concentration and barrier height. The phenomena were explained in terms of the unique bi-phasic microstructures of the material. The research findings reveal valuable microstructural information of temperaturedependent properties of polymer derived ceramics, and should contribute towards more precise understanding and control of the electrical as well as dielectric properties of polymer derivedceramics. Furthermore, the desalination performances and underlying mechanisms of two-dimensional CVD-grown MoS2 layers membranes have been experimentally assessed. Based on a successful large-area few-layer 2D materials growth, transfer and integration method, the 2D MoS2 layers membranes showed preserved chemical and microstructural integrity after integration. The few-layer 2D MoS2 layers demonstrated superior desalination capability towards various types of seawater salt solutions approaching theoretically-predicted values. Such performances are attributed to the dimensional and geometrical effect, as well as the electrostatic interaction of the inherently-present CVD-induced atomic vacancies for governingboth water permeation and ionic sieving at the solution/2D-layer interfaces.
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Date Issued: 2019
Identifier: CFE0007830, ucf:52813
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007830

Title: Design, Synthesis, Stability, and Photocatalytic Studies of Sustainable Metal-Organic Frameworks.
Creator: Logan, Matthew, Uribe Romo, Fernando, Zhai, Lei, Yuan, Yu, Kuebler, Stephen, Rahman, Talat, University of Central Florida
Abstract / Description: The presented dissertation focuses on the design, synthesis, and characterization of metal-organic frameworks (MOFs) composed of earth-abundant elements the exhibit photoredox activity and studied their application as heterogeneous photocatalysts in organic synthesis and in solar-to-chemical energy conversion. In particular, the structure-property relationships of titanium-based MOFs relating the structure of the organic building unit and the photophysical and photochemical activity of the...
Show moreThe presented dissertation focuses on the design, synthesis, and characterization of metal-organic frameworks (MOFs) composed of earth-abundant elements the exhibit photoredox activity and studied their application as heterogeneous photocatalysts in organic synthesis and in solar-to-chemical energy conversion. In particular, the structure-property relationships of titanium-based MOFs relating the structure of the organic building unit and the photophysical and photochemical activity of the solid material is studied. The first novel family of seven MOFs isoreticular to MIL-125-NH2, includes functionalized with N-alkyl groups with increasing chain length (methyl to heptyl) and with varying connectivity (primary or secondary). The functionalized materials displayed reduced optical bandgaps correlated with the increased inductive donor ability of the alkyl substituents, enhanced excited-state lifetimes, mechanistic information towards visible light CO2 reduction, and improved water stability. The second family of titanium MOFs was prepared with a new secondary building unit and organic links of varying lengths, for which Their crystal structure was solved utilizing powder X-ray diffraction crystallography. This work provides guidelines for the next generation of photocatalyst for the conversion of solar-to-chemical energy and other organic transformations.
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Date Issued: 2018
Identifier: CFE0007219, ucf:52217
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007219

Title: Nanoscale Spectroscopy in Energy and Catalytic Applications.
Creator: Ding, Yi, Tetard, Laurene, Challapalli, Suryanarayana, Zhai, Lei, Thomas, Jayan, Lyakh, Arkadiy, Blair, Richard, University of Central Florida
Abstract / Description: Emerging societal challenges such as the need for more sustainable energy and catalysis are requiring more sensitive and versatile measurements at the nanoscale. This is the case in the design and optimization of new materials for energy harvesting (solar cells) and energy storage devices (batteries and capacitors), or for the development of new catalysts for carbon sequestration or other reactions of interest. Hence, the ability to advance spectroscopy with nanoscale spatial resolution and...
Show moreEmerging societal challenges such as the need for more sustainable energy and catalysis are requiring more sensitive and versatile measurements at the nanoscale. This is the case in the design and optimization of new materials for energy harvesting (solar cells) and energy storage devices (batteries and capacitors), or for the development of new catalysts for carbon sequestration or other reactions of interest. Hence, the ability to advance spectroscopy with nanoscale spatial resolution and high sensitivity holds great promises to meet the demands of deeper fundamental understanding to boost the development and deployment of nano-based devices for real applications. In this dissertation, the impact of nanoscale characterization on energy-related and catalytic materials is considered. Firstly an introduction of the current energy and environmental challenges and our motivations are presented. We discuss how revealing nanoscale properties of solar cell active layers and supercapacitor electrodes can greatly benefit the performance of devices, and ponder on the advantages over conventional characterization techniques. Next, we focus on two dimensional materials as promising alternative catalysts to replace conventional noble metals for carbon sequestration and its conversion to added-value products. Defect-laden hexagonal boron nitride (h-BN) has been identified as a good catalyst candidate for carbon sequestration. Theoretically, defects exhibit favorable properties as reaction sites. However, the detailed mechanism pathways cannot be readily probed experimentally, due to the lack of tools with sufficient sensitivity and time resolution. A comprehensive study of the design and material processes used to introduce defects in h-BN in view of improving the catalytic properties is presented. The processing-structure-property relationships are investigated using a combination of conventional characterization and advanced nanoscale techniques. In addition to identifying favorable conditions for defect creation, we also report on the first signs of local reactions at defect sites obtained with nanoscale spectroscopy. Next, we explore avenues to improve the sensitivity and time-resolution of nanoscale measurements using light-assisted AFM-based nanomechanical spectroscopy. For each configuration, we evaluate the new system by comparing its performance to the commercial capabilities.Lastly, we provide a perspective on the opportunities for state-of-the-art characterization to impact the fields of catalysis and sustainable energy, as well as the urge for highly sensitive functional capabilities and time-resolution for nanoscale studies.
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Date Issued: 2018
Identifier: CFE0007751, ucf:52387
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007751

Title: Nitrogen-Containing Materials for Mechanochemical Synthesis, Luminescence Analysis, and Heterogeneous Catalysis.
Creator: Nash, David, Zhai, Lei, Hampton, Michael, Harper, James, Rex, Matthew, Blair, Richard, University of Central Florida
Abstract / Description: Various inorganic nitrogen-containing materials have been exploited for their different properties. Several nitride materials are commercially attractive due to their mechanical properties making them suitable for ceramic industries and wide bandgaps fitting for use as semiconductor and insulator materials, as well as optoelectronics. Nitride materials can exhibit versatility in applications such as the use of gallium nitride to make blue LEDs, nitrides of titanium and silicon being utilized...
Show moreVarious inorganic nitrogen-containing materials have been exploited for their different properties. Several nitride materials are commercially attractive due to their mechanical properties making them suitable for ceramic industries and wide bandgaps fitting for use as semiconductor and insulator materials, as well as optoelectronics. Nitride materials can exhibit versatility in applications such as the use of gallium nitride to make blue LEDs, nitrides of titanium and silicon being utilized as medical implants for their chemical inertness and hardness, and the heavy use of boron nitride as a solid lubricant in the cosmetic industry. Amines have been used as nitrogen-containing organic ligands in organometallic complexes that exhibit phenomenal photophysical properties. These complexes have been heavily studied for potential applications in optoelectronics and chemical sensing. This dissertation will focus on two nitrogen-containing materials that have yet to be explored for the potential applications to be discussed. The first is hexagonal-boron nitride (h-BN), which was previously mentioned to have a substantial use in the cosmetic industry, giving products such as lipstick, foundation, and blush their slick feeling. Computational models have shown the possibility of altered electronic properties of defect sites in the h-BN sheets. These defect sites will be explored experimentally to determine any catalytic activity. Specifically, the hydrogenation reaction using defect-laden hexagonal-boron nitride will be investigated. Successful catalysis would add to the short list of non-metal catalyst, and provide an alternative catalyst that costs significantly less than the traditional metal catalysts commonly used in commercial industries. The second of the two nitrogen-containing materials is a class of metal complexes based on organometallic clusters of copper(I) iodide. Copper(I) iodide clusters formed with amine ligands have been studied for around four decades and the photophysics behind their photoluminescent properties are well understood. Much of the work has been done for use as a potential emissive material in the optoelectronics field. They have also been studied for applications in the sensing of environmental compounds. Here, research will display its use as a novel sensor for narcotic substances. This forensic application will be further explored to develop and eventually commercialize a complete field drug testing system for law enforcement and crime lab use, with the goal to equip law enforcement personnel with a presumptive drug testing method that is accurate, easy-to-use, safe, adaptable, and affordable. This system will consist of a narcotic drug-indicating test strip, a handheld fluorescence spectrometer manufactured in-house using relatively inexpensive parts, and a mobile app that will leverage photoemission data of the tested drug samples collected by multiple crime labs to provide the ability for sample-to-reference data matching. Law enforcement users would have the ability to rapidly identify an unknown substance by applying it to a test strip, testing it using the spectrometer, and capturing an image of the resulting photoemission and analyzing the spectral profile in search of a match with the support of a cloud database.
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Date Issued: 2017
Identifier: CFE0007129, ucf:52297
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007129

Title: Split Aptameric Turn-On Fluorescence Sensor for Detection of Sequence Specific Nucleic Acid.
Creator: Kikuchi, Nanami, Kolpashchikov, Dmitry, Zhai, Lei, Chumbimuni Torres, Karin, Chen, Gang, Teter, Kenneth, University of Central Florida
Abstract / Description: Nucleic acid amplification tests (NAATs) enable sensitive detection of low density infections that microscopy and rapid diagnostic test are not capable of detecting. They enable quantitative and qualitative nucleic acid detection, genotype analysis, and single nucleotide polymorphism (SNP) detection. Current state of the art molecular probes used with NAATs includes molecular beacon (MB), Taqman and its variations. This work presents novel molecular probe designed from Spinach and Dapoxyl...
Show moreNucleic acid amplification tests (NAATs) enable sensitive detection of low density infections that microscopy and rapid diagnostic test are not capable of detecting. They enable quantitative and qualitative nucleic acid detection, genotype analysis, and single nucleotide polymorphism (SNP) detection. Current state of the art molecular probes used with NAATs includes molecular beacon (MB), Taqman and its variations. This work presents novel molecular probe designed from Spinach and Dapoxyl aptamers. The aptamers are split into two parts (split aptamer), allowing greater sensitivity and selectivity towards fully complementary nucleic acid analyte. The major advantage of split aptamer probe over state-of-the-art fluorescent probes is its high selectivity: in the presence of a single base mismatched analyte, it produces only background fluorescence, even at room temperature. SSA is a promising tool for label-free analysis of nucleic acids at ambient temperatures.Split spinach aptamer (SSA) probes and split dapoxyl aptamer (SDA) for fluorescent analysis of nucleic acids were designed and tested. In both split aptamer design, two RNA or RNA/DNA or DNA strands hybridized to a specific nucleic acid analyte and formed a binding site for fluorescent dye, which was accompanied by up to 270-fold and 69-fold increase in fluorescence. SSAr consisted entirely of ribonucleotides which potentially be expressed in live cells and used for imaging of specific mRNAs. For in vitro RNA/DNA analysis, SDA consisting of entirely DNA are preferable due to greater chemical stability, lower synthetic cost and reduced ability to form intramolecular structures. Additionally, we designed two DNA strands that function as an adapter for SSA and demonstrated how a single universal spinach aptamer (USSA) probe can be used to detect multiple (potentially any) nucleic acid sequences. USSA can be used for cost-efficient and highly selective analysis of even folded DNA and RNA analytes, as well as for the readout of outputs of DNA logic circuits.
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Date Issued: 2018
Identifier: CFE0007031, ucf:51976
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007031

Title: Rare Earth Oxide Coating with Controlled Chemistry Using Thermal Spray.
Creator: Singh, Virendra, Seal, Sudipta, Coffey, Kevin, Raghavan, Seetha, Heinrich, Helge, Zhai, Lei, University of Central Florida
Abstract / Description: Cerium oxide (Ceria) at nano scale has gained significant attention due to its numerous technological applications. Ceria in both doped and undoped forms are being explored as oxygen sensor, catalysis, protective coating against UV and corrosion, solid oxide fuel cell (SOFC) electrolyte and newly discovered antioxidant for biomedical applications. Therefore, there is an imminent need of a technology which can provide a cost effective, large scale manufacturing of nanoceria and its subsequent...
Show moreCerium oxide (Ceria) at nano scale has gained significant attention due to its numerous technological applications. Ceria in both doped and undoped forms are being explored as oxygen sensor, catalysis, protective coating against UV and corrosion, solid oxide fuel cell (SOFC) electrolyte and newly discovered antioxidant for biomedical applications. Therefore, there is an imminent need of a technology which can provide a cost effective, large scale manufacturing of nanoceria and its subsequent consolidation, specially using thermal spray.This dissertation aims to develop a scientific understanding towards the development of pure and doped ceria- based coating for a variety of technological applications, from SOFC applications to corrosion resistant coating. Atmospheric plasma spray (APS) and solution precursor plasma spray (SPPS) techniques for the fabrication of nano ceria coating were investigated. For feedstock powder preparation, a spray drying technique was used for the agglomeration of cerium oxide nano particles to achieve high density coating. Deposition efficiencies and coating porosity as a function of processing parameters were analyzed and optimized using a statistical design of experiment model. The coating deposition efficiency was dependent on the plasma temperature and vaporization pressure of the ceria nanoparticles. However, low standoff distance and high carrier gas flow rate were responsible for the improved density upto 86 (&)#177;3%.An alternative novel SPPS technique was studied for a thin film of cerium oxide deposition from various cerium salt precursors in doped and undoped conditions. The SPPS process allows controlling the chemistry of coating at a molecular level. The deposition mechanism by single scan experiments and the effect of various factors on coating microstructure evolution were studied in terms of splats formation. It was found that the precursor salt (nitrate of cerium) with lower thermal decomposition temperatures was suitable for a high density coating. The high concentration and low spray distance significantly improve the splat morphology and reduced porosity (upto 20%). The feasibility of the trivalent cations (Sm 3+ and Gd 3+) doping into cerium oxide lattice in high temperature plasma was discussed and experimentally studied. XRD analysis revealed the nano crystalline characteristic of the coating and lattice expansion due to doping. The extensive transmission electron microscopy, Scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and thermo gravimetric were conducted to evaluate the precursors, and coating microstructure.Due to facial switching between Ce4+ and Ce3+ oxidation state, the cerium oxide surface becomes catalytically active. Thus, the APS ceria coatings were investigated for their applicability under extreme environmental conditions (high pressure and temperature). The air plasma sprayed coated 17-4PH steel was subjected to high pressure (10 Kpsi) and temperature (300 oF) corrosive environment. The coated steel showed continuous improvement in the corrosion resistance at 3.5 wt% NaCl at ambient temperature for three months study whereas, high pressure did not reveal a significant role in the corrosion process, and however, one needs to do further research. The ceria coated steel also revealed the improvement in corrosion protection (by 4 times) compared to the bare steel at low pH, 300 oF and 4000 Psi environment. This study projects the importance of cerium oxide coatings, their fabrication, optimization and applications.
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Date Issued: 2012
Identifier: CFE0004230, ucf:49023
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004230

Title: Electrochemical Studies of Nanoscale Composite Materials as Electrodes in PEM Fuel Cells.
Creator: Anderson, Jordan, Zhai, Lei, Blair, Richard, Hampton, Michael, Zou, Shengli, Seal, Sudipta, University of Central Florida
Abstract / Description: Polymer electrolyte membrane fuel cells (PEMFCs) have recently acquired much attention as alternatives to combustion engines for power conversion. The primary interest in fuel cell technology is the possibility of 60% power conversion efficiency as compared to the 30% maximum theoretical efficiency limited to combustion engines and turbines. Although originally conceived to work with hydrogen as a fuel, difficulties relating to hydrogen storage have prompted much effort in using other fuels....
Show morePolymer electrolyte membrane fuel cells (PEMFCs) have recently acquired much attention as alternatives to combustion engines for power conversion. The primary interest in fuel cell technology is the possibility of 60% power conversion efficiency as compared to the 30% maximum theoretical efficiency limited to combustion engines and turbines. Although originally conceived to work with hydrogen as a fuel, difficulties relating to hydrogen storage have prompted much effort in using other fuels. Small organic molecules such as alcohols and formic acid have shown promise as alternatives to hydrogen in PEMFCs due to their higher stability at ambient conditions. The drawbacks for using these fuels in PEMFCs are related to their incomplete oxidation mechanisms, which lead to the production of carbon monoxide (CO). When carbon monoxide is released in fuel cells it binds strongly to the platinum anode thus limiting the adsorption and subsequent oxidation of more fuel. In order to promote the complete oxidation of fuels and limit poisoning due to CO, various metal and metal oxide catalysts have been used.Motivated by promising results seen in fuel cell catalysis, this research project is focused on the design and fabrication of novel platinum-composite catalysts for the electrooxidation of methanol, ethanol and formic acid. Various Pt-composites were fabricated including Pt-Au, Pt-Ru, Pt-Pd and Pt-CeO2 catalysts. Electrochemical techniques were used to determine the catalytic ability of each novel composite toward the electrooxidation of methanol, ethanol and formic acid. This study indicates that the novel composites all have higher catalytic ability than bare Pt electrodes. The increase in catalytic ability is mostly attributed to the increase in CO poison tolerance and promotion of the complete oxidation mechanism of methanol, ethanol and formic acid. Formulations including bi- and tri-composite catalysts were fabricated and in many cases show the highest catalytic oxidation, suggesting tertiary catalytic effects. The combination of bi-metallic composites with ceria also showed highly increased catalytic oxidation ability. The following dissertation expounds on the relationship between composite material and the electrooxidation of methanol, ethanol and formic acid. The full electrochemical and material characterization of each composite electrode is provided.
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Date Issued: 2012
Identifier: CFE0004510, ucf:49264
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004510

Title: Fire Retardant Polymer Nanocomposites: Materials Design and Thermal Degradation Modeling.
Creator: Zhuge, Jinfeng, Gou, Jihua, Chen, Ruey-Hung, Kapat, Jayanta, Zhai, Lei, University of Central Florida
Abstract / Description: Compared to conventional materials, polymer matrix composites (PMCs) have a number of attractive properties, including light weight, easiness of installation, potential to lower system-level cost, high overall durability, and less susceptibility to environmental deterioration. However, PMCs are vulnerable to fire such that they degrade, decompose, and sometimes yield toxic gases at high temperature. The degradation and decomposition of composites lead to loss in mass, resulting in loss in...
Show moreCompared to conventional materials, polymer matrix composites (PMCs) have a number of attractive properties, including light weight, easiness of installation, potential to lower system-level cost, high overall durability, and less susceptibility to environmental deterioration. However, PMCs are vulnerable to fire such that they degrade, decompose, and sometimes yield toxic gases at high temperature. The degradation and decomposition of composites lead to loss in mass, resulting in loss in mechanical strength.This research aims to improve the structural integrity of the PMCs under fire conditions by designing and optimizing a fire retardant nanopaper coating, and to fundamentally understand the thermal response and post-fire mechanical behavior the PMCs through numerical modeling. Specifically, a novel paper-making process that combined carbon nanofiber, nanoclay, exfoliated graphite nanoplatelet, and ammonium polyphosphate into a self-standing nanopaper was developed. The nanopaper was then coated onto the surface of the PMCs to improve the fire retardant performance of the material. The morphology, thermal stability, flammability, and post-fire flexural modulus of the nanopaper coated-PMCs were characterized. The fire retardant mechanism of the nanopaper coating was studied.Upon successfully improving the structure integrity of the PMCs by the nanopaper coatings, a thermal degradation model that captured the decomposition reaction of the polymer matrix with a second kind boundary condition (constant heat flux) was solved using Finite Element (FE) method. The weak form of the model was constructed by the weighted residual method. The model quantified the thermal and post-fire flexural responses of the composites subject to continuously applied heat fluxes. A temperature dependent post-fire residual modulus was assigned to each element in the FE domain. The bulk residual modulus was computed by assembling the modulus of each element. Based on the FE model, a refined Finite Difference (FD) model was developed to predict the fire response of the PMCs coated with the nanopapers. The FD model adopted the same post-fire mechanical evaluation method. However, unlike the FE model, the flow of the decomposed gas, and permeability and porosity of the composites were taken into account in the refined FD model. The numerical analysis indicated that the thickness and porosity of the composites had a profound impact on the thermal response of the composites.The research funding from the Office of Naval Research (ONR) and Federal Aviation Administration Center of Excellence for Commercial Space Transportation (FAA COE AST) is acknowledged.
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Date Issued: 2012
Identifier: CFE0004263, ucf:49534
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004263

Title: Understanding the Role of Defects in the Radiation Response of Nanoceria.
Creator: Kumar, Amit, Seal, Sudipta, Heinrich, Helge, Cho, Hyoung, Leuenberger, Michael, Zhai, Lei, Devanathan, Ram, University of Central Florida
Abstract / Description: Nanoscale cerium oxide (nanoceria) have shown to possess redox active property , and has been widely studied for potential use in catalysis, chemical-mechanical planarization, bio-medical and solid oxide fuel cell (SOFC), etc. The redox state of nanoceria can be tuned by controlling the defects within the lattice and thus its physical and chemical properties. Perfect ceria lattice has fluorite structure and the research in last decade has shown that oxide and mixed oxide systems with...
Show moreNanoscale cerium oxide (nanoceria) have shown to possess redox active property , and has been widely studied for potential use in catalysis, chemical-mechanical planarization, bio-medical and solid oxide fuel cell (SOFC), etc. The redox state of nanoceria can be tuned by controlling the defects within the lattice and thus its physical and chemical properties. Perfect ceria lattice has fluorite structure and the research in last decade has shown that oxide and mixed oxide systems with pyrochlore and fluorite have better structural stability under high energy radiation. However, the current literature shows a limited number of studies on the effect of high energy radiation on nanoceria. This dissertation aims at understanding the phenomena occurring on irradiation of nanoceria lattice through experiments and atomistic simulation.At first, research was conducted to show the ability to control the defects in nanoceria lattice and understand the effect in tailoring its properties. The defect state of nanoceria was controlled by lower valence state rare earth dopant europium. Extensive materials characterization was done using high resolution transmission electron microscopy (HRTEM), UV-Visible spectroscopy (UV-Vis), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy to understand the effect of dopant chemistry in modifying the chemical state of nanoceria. The defects originating in the lattice and redox state was quantified with increasing dopant concentration. The photoluminescence property of the control and doped nanoceria were evaluated with respect to its defect state. It was observed that defect plays an important role in modifying the photoluminescence property and that it can be tailored in a wide range to control the optical properties of nanoceria.Having seen the importance of defects in controlling the properties of nanoceria, further experiments were conducted to understand the effect of radiation in cerium oxide thin films of different crystallinity. The cerium oxide thin films were synthesized using oxygen plasma assisted molecular beam epitaxy (OPA-MBE) growth. The thin films were exposed to high energy radiation over a wide range of fluence (1013 to 1017 He+ ions/cm3). The current literature does not report the radiation effect in nanoceria in this wide range and upto this high fluence. The chemical state of the thin film was studied using in-situ XPS for each dose of radiation. It was found that radiation induced defects within both the ceria thin films and the valence state deviated further towards non-stoichiometry with radiation. The experimental results from cerium oxide thin film irradiation were studied in the light of simulation. Classical molecular dynamics and Monte Carlo simulation were used for designing the model ceria nanoparticle and studying the interaction of the lattice model with radiation. Electronic and nuclear stopping at the end of the range were modeled in ceria lattice using classical molecular dynamics to simulate the effect of radiation. It was seen that displacement damage was the controlling factor in defect production in ceria lattice. The simulation results suggested that nanosized cerium oxide has structural stability under radiation and encounters radiation damage due to the mixed valence states. A portion of the study will focus on observing the lattice stability of cerium with increasing concentration of the lower valence (Ce3+) within the lattice. With this current theoretical understanding of the role of redox state and defects during irradiation, the surfaces and bulk of nanoceria can be tailored for radiation stable structural applications.
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Date Issued: 2012
Identifier: CFE0004396, ucf:49375
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004396

Title: Nanoarchitectured Energy Storage Devices.
Creator: Yu, Zenan, Thomas, Jayan, Seal, Sudipta, Zhai, Lei, Fang, Jiyu, Sundaram, Kalpathy, University of Central Florida
Abstract / Description: Supercapacitors, the devices that connect the gap between batteries and conventional capacitors, have recently attracted significant attention due to their high specific capacitance, substantially enhanced power and energy densities, and extraordinary cycle life. In order to realize even better performance with supercapacitors, rejuvenated effort towards developing nanostructured electrodes is necessary. In this dissertation, several strategic directions of nanoarchitecturing the electrodes...
Show moreSupercapacitors, the devices that connect the gap between batteries and conventional capacitors, have recently attracted significant attention due to their high specific capacitance, substantially enhanced power and energy densities, and extraordinary cycle life. In order to realize even better performance with supercapacitors, rejuvenated effort towards developing nanostructured electrodes is necessary. In this dissertation, several strategic directions of nanoarchitecturing the electrodes to enhance the performance of supercapacitors are investigated. An introduction and background of supercapacitors, which includes motivation, classification and working principles, recent nanostructured electrode materials studies, and devices fabrication, are initially presented. A facile method, called Spin-on Nanoprinting (SNAP), to fabricate highly ordered manganese dioxide (MnO2) nanopillars is introduced. The SNAP method that is further modified to develop carbon nanoarray electrodes is also discussed. Subsequently, a template-free method to develop high aspect ratio copper oxide nanowhiskers on copper substrate is presented, which boosts the surface area by 1000 times compared to non-nanostructured copper substrate. Electrochemically deposited MnO2 on the nanostructured substrate provided a specific capacitance of about 1379 F g-1 which is very close to the theoretical value (~ 1400 F g-1) due to this efficient nanostructure design. In addition, a novel method to decorate metal nanoparticles on graphene aerogel, which considerably enhances the electronic conductivity and the corresponding specific capacitance, is demonstrated. Moreover, ferric oxide (Fe2O3) nanorods prepared by a simple hydrothermal method is discussed. Asymmetric devices assembled based on Fe2O3 nanorods and MnO2 nanowhiskers show excellent electrochemical properties. The devices not only display the capability to store energy but also transmit electricity through the inner copper core. These two functions are independent and do not interfere with each other. Finally, a summary of this dissertation as well as some potential future directions are presented.
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Date Issued: 2015
Identifier: CFE0006062, ucf:50995
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0006062

Title: Electronic Structure of Metal (Al, Cu) Doped Carbon Nanotubes and the Resultant Conduction of the Hybrid Materials.
Creator: Jiang, Jingyin, Chen, Quanfang, Zhai, Lei, Fang, Jiyu, Bai, Yuanli, Stolbov, Sergey, University of Central Florida
Abstract / Description: Due to the exceptional strength, stiffness and excellent electrical and thermal properties, carbon nanotubes (CNTs) have been regarded as promising candidates for advanced nanoelectronics and multifunctional nanocomposites. In this dissertation, the interaction of CNTs with metals have been investigated and the resultant electrical conduction have been analyzed, aiming to develop innovative avenues to best utilize CNTs' potential. In order to do so, quantum mechanics calculations have been...
Show moreDue to the exceptional strength, stiffness and excellent electrical and thermal properties, carbon nanotubes (CNTs) have been regarded as promising candidates for advanced nanoelectronics and multifunctional nanocomposites. In this dissertation, the interaction of CNTs with metals have been investigated and the resultant electrical conduction have been analyzed, aiming to develop innovative avenues to best utilize CNTs' potential. In order to do so, quantum mechanics calculations have been carried out to study that how to obtain greater electrical conduction by doping metals (Cu, Al) which tailor the electronic structure of three different types of metal-CNT interactions, : 1) encapsulation of atoms inside the CNTs, 2) adsorption of atoms onto CNT surface, and 3) substitutional doping. Models of different doping methods were built and optimized with Density Functional Theory (DFT). And in conjunction with non-equilibrium Green's function, the electronic structure and the conducting properties were then calculated.Through this study, both metallic and semiconducting CNTs have been used. Metallic CNT (5, 5) encapsulated with copper chains have been first investigated with an emphasis on the electronic structure and the resultant conductance. The Density of States (DOS) have showed that the encapsulation of Cu effectively introduced more states around the fermi level. And due to the interaction between copper and CNTs, the conductance of the metallic CNTs-Cu system can be significantly increased.In addition to copper, aluminum has been also introduced for the study. The electronic structure and transport properties of hybrid nanowires consisting of aluminum chains adsorbed on a single-wall semiconducting CNT (10, 0) have been calculated. The band structure and DOS of the hybrid nanowires have showed that the adsorption of Al can effectively reduce the band gap. And with more than 4 Al chains adsorbed, the CNT has transformed from semiconducting to conducting. The transmission eigenstates further indicated that both Al chains and the modified nanotube were responsible for the increased conduction in the hybrid nanowires. The resultant conductance of CNT (10, 0)/Al hybrid nanowire is about 40% greater than that of pure Cu nanowire with the same diameter. In order to utilize the extraordinary conductance in CNT(10,0)/Al hybrid nanowire, it is also important to investigate the end-contact between the hybrid nanowire with Al electrodes. During this work the transmission spectrum at different bias voltage were calculated to study the I-V characteristics and the electrical contact resistances at the interfaces. The results have suggested that the electrical contact resistances between Al electrodes and the hybrid nanowire is significantly lower than that of Al-pure CNT contacts, although the actual contact resistance is directional dependent that the contact resistance is reduced to 20% of that Al-pure CNT along the longitudinal direction.The possibility of substitutional doping of Cu and Al in both metallic and semiconducting CNTs were also investigated. The formation energies have showed that Al doping was more energy favorable than Cu doping in both cases. And by doping of Al or Cu, a metallic tube experienced a higher conductance and a semiconducting tube has transited to conducting.In summary, different doping methods could modify the conducting property of nanotubes. Encapsulation of Cu in metallic CNT results in a significant conductance increment. Adsorption of Al transforms semiconducting CNT to conducting and reduces the contact resistance between the nanowire and Al electrode. Substitutional doping of Cu or Al transits semiconducting nanotube to conducting and enhance the conductance of metallic nanotube.
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Date Issued: 2017
Identifier: CFE0006607, ucf:51274
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0006607

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