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Development of enzyme-free hydrogen peroxide biosensor using cerium oxide and mechanistic study using in-situ spectro-electrochemistry
Title
Development of enzyme-free hydrogen peroxide biosensor using cerium oxide and mechanistic study using in-situ spectro-electrochemistry.
Creator
Saraf, Shashank, Seal, Sudipta, Cho, Hyoung Jin, Zhai, Lei, Heinrich, Helge, Harper, James, University of Central Florida
Abstract / Description
During recent development, it has been demonstrated that cerium oxide nanoparticles (CNPs) have exhibited catalytic activity which mimics naturally existing enzymes such as superoxide dismutase (SOD) and catalase. The underlying mechanism is attributed to the modulation of oxygen vacancies on CNPs lattice by dynamic switching of the oxidation states between Ce3+ and Ce4+ due to the electron transfer resulting from the redox reaction between CNPs and reactive oxygen species such as hydrogen...
Show moreDuring recent development, it has been demonstrated that cerium oxide nanoparticles (CNPs) have exhibited catalytic activity which mimics naturally existing enzymes such as superoxide dismutase (SOD) and catalase. The underlying mechanism is attributed to the modulation of oxygen vacancies on CNPs lattice by dynamic switching of the oxidation states between Ce3+ and Ce4+ due to the electron transfer resulting from the redox reaction between CNPs and reactive oxygen species such as hydrogen peroxide (H2O2). Thereby the redox potential of CNPs is dependent on the surface chemistry i.e. the surface concentration of Ce3+ and Ce4+ Currently, the ratio of Ce3+/ Ce4+ in CNPs is characterized ex-situ using XPS or TEM which involves sample drying and exposure to high energy X-rays and electron beam, respectively. Sample drying and high energy beam exposure could lead to sample deterioration. The goal of the study is to explore a technique to characterize CNPs in-situ and identify the surface chemistry of CNPs. The in-situ investigation of CNPs was carried using spectroelectrochemistry wherein the electrochemical and optical measurements are carried out simultaneously. Detailed optical characterization of two different CNPs having different catalytic activity were carried under oxidation and reduction environments. Analysis of spectra revealed widely different redox potential for CNPs which was a function of pH and composition of buffer solution. In second part of dissertation a suitable surface chemistry of CNPs is investigated to replace the enzyme in biosensor assembly to allow amperometric detection of H2O2 in physiological conditions. Upon electrochemical investigation of the physio-chemical properties of CNPs, it was found that CNPs having higher surface concentration of Ce4+ as compared to Ce3+ oxidation states, demonstrated increased catalytic activity towards H2O2. The addition of CNPs resulted in 5 orders of increment in amperometric current with a response time of 400 msec towards detection of H2O2 and exhibited excellent selectivity in presence of interfering species. Additionally, cerium oxide was successfully integrated into the biosensor assembly through the anodic electrodeposition, which allowed the transfer of electron generated from the CNPs in the redox reaction to the electrode and demonstrated successful sensing of H2O2. Furthermore, to achieve detection of H2O2 in physiological conditions, CNPs were integrated with nanoporous gold (NPG) which exhibited anti-biofouling properties. The anti-biofouling property of NPG was investigated using electrochemical techniques and showed excellent signal retention in physiological concentration of albumin proteins. The novel study targets at developing robust enzyme free biosensor by integrating the detection ability of CNPs with the anti-biofouling activity of NPG based electrode.
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Date Issued
2016
Identifier
CFE0006498, ucf:51404
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006498
Manufacturing of Single Solid Oxide Fuel Cells
Title
Manufacturing of Single Solid Oxide Fuel Cells.
Creator
Torres-Caceres, Jonathan, Orlovskaya, Nina, Xu, Yunjun, Das, Tuhin, University of Central Florida
Abstract / Description
Solid oxide fuel cells (SOFCs) are devices that convert chemical energy into electrical energy and have the potential to become a reliable renewable energy source that can be used on a large scale. SOFCs have 3 main components; the electrolyte, the anode, and the cathode. Typically, SOFCs work by reducing oxygen at the cathode into O2- ions which are then transported via the electrolyte to the anode to combine with a fuel such as hydrogen to produce electricity. Research into better materials...
Show moreSolid oxide fuel cells (SOFCs) are devices that convert chemical energy into electrical energy and have the potential to become a reliable renewable energy source that can be used on a large scale. SOFCs have 3 main components; the electrolyte, the anode, and the cathode. Typically, SOFCs work by reducing oxygen at the cathode into O2- ions which are then transported via the electrolyte to the anode to combine with a fuel such as hydrogen to produce electricity. Research into better materials and manufacturing methods is necessary to reduce costs and improve efficiency to make the technology commercially viable.The goal of the research is to optimize and simplify the production of single SOFCs using high performance ceramics. This includes the use of 8mol% Y2O3-ZrO2 (YSZ) and 10mol% Sc2O3-1mol%CeO2-ZrO2 (SCSZ) layered electrolytes which purport higher conductivity than traditional pure YSZ electrolytes. Prior to printing the electrodes onto the electrolyte, the cathode side of the electrolyte was coated with 20mol% Gd2O3-CeO2 (GDC). The GDC coating prevents the formation of a nonconductive La2Zr2O7 pyrochlore layer, which forms due to the interdiffusion of the YSZ electrolyte ceramic and the (La0.6Sr0.4)0.995Fe0.8Co0.2O3 (LSCF) cathode ceramic during sintering. The GDC layer was deposited by spin coating a suspension of 10wt% GDC in ethanol onto the electrolyte. Variation of parameters such as time, speed, and ramp rate were tested. Deposition of the electrodes onto the electrolyte surface was done by screen printing. Ink was produced using a three roll mill from a mixture of ceramic electrode powder, terpineol, and a pore former. The pore former was selected based on its ability to form a uniform well-connected pore matrix within the anode samples that were pressed and sintered. Ink development involved the production of different ratios of powder-to-terpineol inks to vary the viscosity. The different inks were used to print electrodes onto the electrolytes to gauge print quality and consistency. Cells were produced with varying numbers of layers of prints to achieve a desirable thickness. Finally, the densification behaviors of the major materials used to produce the single cells were studied to determine the temperatures at which each component needs to be sintered to achieve the desired density and to determine the order of electrode application, so as to avoid over-densification of the electrodes. Complete cells were tested at the National Energy Technology Laboratory in Morgantown, WV. Cells were tested in a custom-built test stand under constant voltage at 800(&)deg;C with 3% humidified hydrogen as the fuel. Both voltage-current response and impedance spectroscopy tests were conducted after initial startup and after 20 hours of operation. Impedance tests were performed at open circuit voltage and under varying loads in order to analyze the sources of resistance within the cell. A general increase in impedance was found after the 20h operation. Scanning electron micrographs of the cell microstructures found delamination and other defects which reduce performance. Suggestions for eradicating these issues and improving performance have been made.
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Date Issued
2013
Identifier
CFE0004946, ucf:49641
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0004946
SLURRY CHEMISTRY EFFECTS ON COPPER CHEMICAL MECHANICAL PLANARIZATION
Title
SLURRY CHEMISTRY EFFECTS ON COPPER CHEMICAL MECHANICAL PLANARIZATION.
Creator
Luo, Ying, Desai, Vimal, University of Central Florida
Abstract / Description
ABSTRACTChemical-mechanical Planarization (CMP) has emerged as one of the fastest-growing processes in the semiconductor manufacturing industry, and it is expected to show equally explosive growth in the future (Braun, 2001). The development of CMP has been fueled by the introduction of copper interconnects in microelectronic devices. Other novel applications of CMP include the fabrications of microelectromechanical systems (MEMS), advanced displays, three dimensional systems, and so on ...
Show moreABSTRACTChemical-mechanical Planarization (CMP) has emerged as one of the fastest-growing processes in the semiconductor manufacturing industry, and it is expected to show equally explosive growth in the future (Braun, 2001). The development of CMP has been fueled by the introduction of copper interconnects in microelectronic devices. Other novel applications of CMP include the fabrications of microelectromechanical systems (MEMS), advanced displays, three dimensional systems, and so on (Evans, 2002). CMP is expected to play a key role in the next-generation micro- and nanofabrication technologies (Singh, et al., 2002).Despite the rapid increase in CMP applications, the fundamental understanding of the CMP process has been lacking, particularly the understanding of the wafer-slurry-pad interactions that occur during the CMP process. Novel applications of CMP are expected to expand to materials that are complex chemically and fragile mechanically. Thus, fundamental understanding and improvement of slurry design for CMP is the key to the development of sophisticated next-generation CMP processes.Slurry performance for CMP can be determined by several output parameters including removal rate, global planarity, surface topography, and surface defectivity. To achieve global planarity, it is essential to form a very thin passivating surface layer (<2 nm) that is subsequently removed by the mechanical component of the slurry (Kaufman et al., 1991) or by combined chemo-mechanical effects (Tamboli, 2000). Chemical additives like hydrogen peroxide (H2O2), potassium ferricyanide, and ferric chloride are added to slurries as oxidizers in order to form a desirable surface layer. Other chemical additives such as inhibitors (e.g. benzotriazole) and complexing agents (e.g. ammonia) are added to the copper slurry in order to modify the oxide layer. That the removal rate of the thin surface layer is greater at the highest regions of the wafer surface than at the lowest regions leads to surface planarity.In this study, various complexing agents and inhibitors are combined to form slurry chemistry for copper CMP processing in H2O2 based slurries at pH values ranging from 2 to 10. Two complexing agents (glycine and Ethylenediamine) and one inhibitor (3-amino-1, 2, 4-triazole) were selected as slurry constituents for detailed chemical synergistic effect study because they showed good materials removal and surface planarity performances.To understand the fundamental mechanisms involved in copper CMP process with the afore-mentioned slurry chemical formations, various techniques, such as electrochemical testing techniques (including potentiodynamic polarization and electrochemical impedance spectroscopy), x-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), and scanning electron microscopy (SEM), were applied. As a result, guidelines for optimized slurry chemical formulation were arrived at and the possible mechanisms of surface-chemical-abrasive interactions were determined. From applications point of view, this study serves as a guide for further investigations in pursuing highly effective slurry formulations for copper/low-k interconnect applications.
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Date Issued
2004
Identifier
CFE0000120, ucf:46195
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0000120
Synthetic Design and Characterization of Polycyclic Aromatic Compounds in Molecular and Extended System
Title
Synthetic Design and Characterization of Polycyclic Aromatic Compounds in Molecular and Extended System.
Creator
Pour, Gavin, Belfield, Kevin, Frazer, Andrew, Elsheimer, Seth, University of Central Florida
Abstract / Description
The work presented herein focuses on the synthesis and characterization of polycyclic aromatic compounds for a wide variety of toxicological, analytical, and electronic applications. First, the modular synthesis of 12 dibenzo- and naphtho- fluoranthene polycyclic aromatic hydrocarbons (PAHs) via a Pd-catalyzed five-membered ring closing procedure is discussed. By understanding the various modes through which the Pd migrates during transformation, structural rearrangements were bypassed,...
Show moreThe work presented herein focuses on the synthesis and characterization of polycyclic aromatic compounds for a wide variety of toxicological, analytical, and electronic applications. First, the modular synthesis of 12 dibenzo- and naphtho- fluoranthene polycyclic aromatic hydrocarbons (PAHs) via a Pd-catalyzed five-membered ring closing procedure is discussed. By understanding the various modes through which the Pd migrates during transformation, structural rearrangements were bypassed, obtaining regioselectivity through various redesigns in the synthetic route. Each compound in the serious was rigorously characterized via 1D/2D NMR, absorption and emission spectroscopy as well as cyclic voltammetry, which shows vast differences due to small structural changes between these constitutional isomers. Next, a series of polyphenylated organic ligands for zirconium metal organic frameworks is presented as materials for post-synthetic Scholl cyclodehydrogenation. Lastly, a series of organic linkers featuring covalently anchored redox-active pendants is explored for tuneable redox activity in Zr-based metal-organic frameworks. Thin-films were grown onto fluorine-doped tin-oxide glass electrodes and analyzed by cyclic voltammetry. This is the first reported pre-synthetic incorporation of covalently-bound ferrocenyl pendants into such a system. By attenuating the proportions of redox active and inactive links the oxidative peak currents could be tuned. This body of work represents a contribution toward the practical design and synthesis of polycyclic aromatic for a wide variety of analytical and electrochemical applications.
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Date Issued
2019
Identifier
CFE0007512, ucf:52647
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0007512
INVESTIGATION OF NANOCERIA-MODIFIED PLATINUM-GOLD COMPOSITE ELECTRODES FOR THE ELECTROCHEMICAL REDUCTION OF OXYGEN IN ALKALINE MEDIA
Title
INVESTIGATION OF NANOCERIA-MODIFIED PLATINUM-GOLD COMPOSITE ELECTRODES FOR THE ELECTROCHEMICAL REDUCTION OF OXYGEN IN ALKALINE MEDIA.
Creator
Hegishte, Rahul, Diaz, Diego, University of Central Florida
Abstract / Description
Platinum-gold and nanoceria-modified platinum-gold electrodes were prepared on a platinum surface via electrochemical reduction of solutions of platinum and gold salts in the dispersion of nanoceria. The molar ratios of Pt and Au were varied in both PtAu and PtAu/CeO2 electrodes while the total concentration of the metals was maintained at 2 x 10-3M and the concentration of nanoceria was maintained constant at 5 x 10-3M. The electrodes were characterized by their cyclic voltammetry curves in...
Show morePlatinum-gold and nanoceria-modified platinum-gold electrodes were prepared on a platinum surface via electrochemical reduction of solutions of platinum and gold salts in the dispersion of nanoceria. The molar ratios of Pt and Au were varied in both PtAu and PtAu/CeO2 electrodes while the total concentration of the metals was maintained at 2 x 10-3M and the concentration of nanoceria was maintained constant at 5 x 10-3M. The electrodes were characterized by their cyclic voltammetry curves in 0.5M sulfuric acid solution. The electrochemically active area of the electrodes was determined using the copper underpotential deposition method. The linear sweep voltammograms of the PtAu and PtAu/CeO2 electrodes were plotted from -1V to 0V vs. Ag/AgCl, 3M KCl reference electrode using the rotating disk electrodes for the rotation speeds from 200 to 3600rpm in an oxygen saturated 0.1M sodium hydroxide solution. The values of the kinetic controlled current density were determined from the rotating disk voltammetry. The values of the limiting current density for each rotation speed were used to plot the Koutecky-Levich plots for the electrodes. The rate constants were obtained from the Koutecky-Levich plots for each composition of the electrode. The values of kinetic current density and the rate constants indicated that the addition of Au enhances the ORR rates in both the PtAu and the PtAu/CeO2 electrodes. The values of the kinetic current densities of the PtAu/CeO2 were lower than that of the PtAu electrodes owing to the poor electrical conductivity of ceria. The Koutecky-Levich plots for the PtAu and the PtAu/CeO2 electrodes are linear for the four-electron reduction of oxygen in the alkaline media, which indicates that the overall reaction follows the first order kinetics. The electron transfer rate constants obtained from the Koutecky-Levich plots for the PtAu and the PtAu/CeO2 electrodes both were found to increase in values with the addition of Au. The Tafel plots were plotted for the PtAu and PtAu/CeO2 electrodes and the values of Tafel slopes were found to be in a small range for lower amounts of Au which indicated that the ORR rates were enhanced in lower amounts of Au. The values of Tafel slopes were found to be much higher for the ceria-modified PtAu electrodes as compared to the PtAu electrodes, which indicate the lower rates of ORR after the modification with ceria. Also, the ORR rates for the electrodes with smaller amounts of Au in PtAu/CeO2 were higher than those in the larger amounts of Au.
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Date Issued
2011
Identifier
CFE0003639, ucf:48860
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0003639