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(1 - 9 of 9)
- Title
- SOLUTION PROCESSIBLE AROMATIC POLYIMIDES VIA DIELS ALDER PRECURSOR.
- Creator
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Shah, Saral, Liao, Yi, University of Central Florida
- Abstract / Description
-
Aromatic polyimides are interesting materials since they possess outstanding key properties such as thermoxidative stability, high mechanical strength, high modulus, excellent electrical properties, and superior chemical resistance. However, their low solubility makes them difficult to characterize, process and obtain high molecular weight polymer. In this report, we synthesized a series of precursor polymers that contains Diels-Alder (DA) adducts of anthracene. Different dienophiles were...
Show moreAromatic polyimides are interesting materials since they possess outstanding key properties such as thermoxidative stability, high mechanical strength, high modulus, excellent electrical properties, and superior chemical resistance. However, their low solubility makes them difficult to characterize, process and obtain high molecular weight polymer. In this report, we synthesized a series of precursor polymers that contains Diels-Alder (DA) adducts of anthracene. Different dienophiles were tried. These precursor polymers are soluble in common organic solvents such as chloroform and can be easily processed to thin films. Heating the film above 215 degree induce retro-DA reaction, which generated the fully aromatic polyimides in situ. The solid-state retro-DA reactions were monitored by ATR-FTIR and UV-Vis spectra. The fully aromatic polyimides are highly stable and their thin films are insoluble in organic solvents. Profilometry and AFM studies showed that after the thermal treatment, the films are smooth and pin-hole free, while the volumes decreased with a percentage close to the weight loss caused by retro-DA reaction. These Polymers can have a wide range of potential applications from thermal patterning polymers to organic photovoltaics.
Show less - Date Issued
- 2008
- Identifier
- CFE0002387, ucf:47735
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0002387
- Title
- PHOTO RETRO DIELS-ALDER REACTION OF THE ADDUCTS OF TETRACYANOETHYLENE AND POLYAROMATIC COMPOUNDS.
- Creator
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Banerjee, Siddthartha, Liao, Yi, University of Central Florida
- Abstract / Description
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Thermally induced retro-Diels Alder (rDA) reaction has been extensively used for the preparation of many reactive intermediates in organic synthesis. But the uses of photo-retro Diels-Alder (PrDA) reaction in organic synthesis were sparingly reported in literature. Due to its spatial and temporal control, PrDA can be used in making of photosensitive materials, in drug delivery and also for mechanistic studies. Diels-Alder adducts of tetracyanoethylene (TCNE) and polyaromatic compounds ...
Show moreThermally induced retro-Diels Alder (rDA) reaction has been extensively used for the preparation of many reactive intermediates in organic synthesis. But the uses of photo-retro Diels-Alder (PrDA) reaction in organic synthesis were sparingly reported in literature. Due to its spatial and temporal control, PrDA can be used in making of photosensitive materials, in drug delivery and also for mechanistic studies. Diels-Alder adducts of tetracyanoethylene (TCNE) and polyaromatic compounds (anthracene, napthacene, pentacene and phencyclone) were synthesized and were subjected to PrDA reaction through 254-nm irradiation. The quantum yield and the consequent photoreactivity of these DA adducts follow the following order. TCNE/naphthacene > TCNE/anthracene > TCNE/pentacene This trend was explained by a mechanism of charge-separated intermediates. The stability of the charge-separated intermediate is the governing factor of this trend of photoractivity of DA adducts. Based on these results it is possible to design a proper DA adduct and consequently predict the feasibility of the PrDA reaction.
Show less - Date Issued
- 2011
- Identifier
- CFE0004029, ucf:49165
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004029
- Title
- Photochemistry and Applications of Diels-Alder Adducts and Photoacids in Materials Science.
- Creator
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Johns, Valentine, Liao, Yi, Miles, Delbert, Zou, Shengli, Gesquiere, Andre, Su, Ming, University of Central Florida
- Abstract / Description
-
Utilizing light as an energy source for reactions has intrigued many chemists. This has led to the development of the principles of photochemistry. The Photo retro Diels Alder (PrDA) reaction is one such system that has potential for use in materials science as well as in the life sciences. However, there was no guide to predict whether a compound could undergo the PrDA reaction, which limits the widespread use of this reaction. Another system is that of photoacids (molecules that release...
Show moreUtilizing light as an energy source for reactions has intrigued many chemists. This has led to the development of the principles of photochemistry. The Photo retro Diels Alder (PrDA) reaction is one such system that has potential for use in materials science as well as in the life sciences. However, there was no guide to predict whether a compound could undergo the PrDA reaction, which limits the widespread use of this reaction. Another system is that of photoacids (molecules that release protons upon irradiation reversibly). Since most fundamental processes involve proton transfer, these types of photoacids have great potential which is yet to be explored. This thesis describes the design and synthesis of various aromatic DA adducts. These adducts were made to undergo the rDA reaction using UV (Ultra-Violet) light. Experimental results showed that the photoreactivity of these adducts depends on the electron-donating ability of the diene component and the electron-withdrawing ability of the dienophile component. In addition, mechanistic study of this reaction revealed the formation of a charge separated intermediate with a singlet excited state. The potential of the PrDA reaction was also explored in two ways. One was by designing isomeric DA adducts from pentacene and TCNE (tetracyanoethylene) which are capable of switching from one isomer to another via a PrDA process. The other way was the design and synthesis of a polymer with an anthracene diketone moeity which could undergo a PrDA reaction to change from an insulator to a semiconductor. Finally, the syntheses of a number of photoacids which not only become acidic upon irradiation but also respond to visible light reversibly have been explored. A rationale has been developed for the design of photoacids with desired photo-induced response. While electron donating and accepting groups in strategic positions help tune the pH; using different combinations of ethanol and water affect the rate of the forward and the backward processes. A photoacid monomer was also incorporated into three photoacid polymers which respond to visible light reversibly, hence promising widespread applications of these photoacids.
Show less - Date Issued
- 2012
- Identifier
- CFE0004556, ucf:49235
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004556
- Title
- Electrical, Optical and Chemical Properties of Organic Photo Sensitve Materials.
- Creator
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Shi, Zheng, Liao, Yi, Kolpashchikov, Dmitry, Ye, Jingdong, Zou, Shengli, Su, Ming, University of Central Florida
- Abstract / Description
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Light as a (")green(") source of energy has become increasingly attractive throughout the past century and has shown versatility for the application of activating chemical reactions. Compared with traditional energy sources, it provides a more direct, selective and controllable method. My PhD study was focused on the study of photochemistry of organic materials in two different systems. The first system is regarding reversible photoacids which generate protons on irradiation. With the aim of...
Show moreLight as a (")green(") source of energy has become increasingly attractive throughout the past century and has shown versatility for the application of activating chemical reactions. Compared with traditional energy sources, it provides a more direct, selective and controllable method. My PhD study was focused on the study of photochemistry of organic materials in two different systems. The first system is regarding reversible photoacids which generate protons on irradiation. With the aim of systematically studying these novel types of long lived photoacids, a series of photoacids was designed, synthesized and whose chemical mechanism was thoroughly investigated. This type of photoacid changes from a weak acid to a strong acid with a pH change of several units, which achieves nearly complete proton dissociation upon visible light irradiation. The whole process is reversible and the half-life of the proton-dissociation state is long enough to be used in many applications. Besides fundamental studies, different applications based on this type of photoacids were also completed. An esterification reaction was catalyzed and the volume of a pH-sensitive polymer was altered due to the large amount of photo generated protons from this photoacid. A reversible electrical conductivity change of polyaniline (PANI) was also achieved by doping with this reversible photoacid. In order to induce a large conductivity increase, an irreversible photoacid generator (PAG) was embedded in a novel PANI/PAG/PVA novel composition. In this system, Poly (vinyl alcohol) (PVA) forms a hydrogen-bonding network to facilitate proton transfer between the PAG and PANI. A final electrical conductivity of 10-1 S cm-1 was successfully achieved after irradiation. The second system in which I explored photochemistry of organic molecules concerns Photo-retro-Diels-Alder (PrDA) reactions and a variety of Diels-Alder (DA) adducts were designed for these studies. UV light was used to trigger the retro-Diels-Alder reactions. Quantum yield of each DA adducts was investigated. This revealed that the photo-reactivity of this process depends on the electron-donating ability of the diene and the electron-withdrawing ability of the dienophile component. Mechanistic studies of this PrDA reaction reveal that a charge-separated intermediate is generated from a singlet excited state. This was applied to an unsaturated cyclic ?-diketones (DKs), which underwent PrDA reactions and generated anthracene derivatives and carbon monoxide (CO), which itself plays profound and important roles in biological systems. These unsaturated cyclic ?-diketones (DKs) encapsulated in micelles are effective CO-releasing molecules (CORMs) and are capable of carrying and releasing CO in cellular systems. This novel type of organic CORMs has potentially low toxicity and generates fluorescence, which provides a useful tool for the study of the biological functions of CO.
Show less - Date Issued
- 2013
- Identifier
- CFE0005114, ucf:50748
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005114
- Title
- On the Capillary Electrophoresis of Monohydroxy Metabolites of Polycyclic Aromatic Hydrocarbons and its Application to the Analysis of Biological Matrices.
- Creator
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Knobel, Gaston, Campiglia, Andres, Clausen, Christian, Belfield, Kevin, Liao, Yi, Bhattacharya, Aniket, University of Central Florida
- Abstract / Description
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Polycyclic aromatic hydrocarbons (PAH) are a class of environmental pollutants consisting of a minimum of two fused aromatics rings originating from the incomplete combustion of organic matter and/or anthropogenic sources. Numerous possible anthropogenic and natural sources make the presence of PAH ubiquitous in the environment. The carcinogenic nature of some PAH and their ubiquitous presence makes their chemical analysis a topic of environmental and toxicological importance. Although...
Show morePolycyclic aromatic hydrocarbons (PAH) are a class of environmental pollutants consisting of a minimum of two fused aromatics rings originating from the incomplete combustion of organic matter and/or anthropogenic sources. Numerous possible anthropogenic and natural sources make the presence of PAH ubiquitous in the environment. The carcinogenic nature of some PAH and their ubiquitous presence makes their chemical analysis a topic of environmental and toxicological importance. Although environmental monitoring of PAH is an important step to prevent exposure to contaminated sites, it provides little information on the actual uptake and subsequent risks. Parent PAH are relatively inert and need metabolic activation to express their carcinogenicity. Covalent binding to DNA appears to be the first critical step in the initiation of the tumor formation process.To this end, the determination of short term biomarkers (-) such as monohydroxy-PAH metabolites (OH-PAH) - fills an important niche to interpret actual PAH exposure levels, prevent extreme body burdens and minimize cancer risk. One would certainly prefer an early warning parameter over a toxicological endpoint (-) such as DNA-adducts (-) indicating that extensive damage has already been done. Several methods have been developed to determine OH-PAH in specific tissue or excreta and food samples. The general trend for the analysis of OH-PAH follows the pattern of sample collection, sample clean-up and pre-concentration, chromatographic separation and quantification. Popular approaches for sample clean-up and pre-concentration include liquid-liquid extraction (LLE) and solid-phase extraction (SPE). Chromatographic separation and quantification has been based on high-performance liquid chromatography-room temperature fluorescence detection (HPLC) and gas chromatography-mass spectrometry (GC-MS).Although chromatographic techniques provide reliable results in the analysis of OH-PAH, their experimental procedures are time consuming and expensive. Elution times of 30-60 minutes are typical and standards must be run periodically to verify retention times. If the concentrations of target species are found to lie outside the detector's response range, the sample must be diluted and the process repeated. On the other end of the concentration range, many samples are (")zeroes,(") i.e. the concentrations are below detection limits. Additional problems arise when laboratory procedures are scaled up to handle thousands of samples under mass screening conditions. Under the prospective of a sustainable environment, the large usage of organic solvents is one of the main limitations of the current chromatographic methodology.This dissertation focuses on the development of a screening methodology for the analysis of OH-PAH in urine and milk samples. Screening techniques capable of providing a (")yes or no(") answer to OH-PAH contamination prevent unnecessary scrutiny of un-contaminated samples via conventional methods, reduce analysis cost and expedite the turnaround time for decision making purposes. The proposed methodology is based on capillary zone electrophoresis (CZE) and synchronous fluorescence spectroscopy (SFS). Metabolites extraction and pre-concentration is achieved with optimized SPE, LLE and/or QuEChERS (quick, easy, cheap, effective, rugged and safe) procedures. The small sample and extracting solvent volumes facilitate the simultaneous extraction of numerous samples via an environmentally friendly procedure, which is well-suited for routine monitoring of numerous samples. Sample stacking is successfully implemented to improve CZE limits of detection by two orders of magnitude. The unique electrophoretic pattern of positional isomers of OH-PAH demonstrates the potential of CZE for the unambiguous determination of metabolites with similar chromatographic behaviors and virtually similar fragmentation patterns. The direct determination of OH-PAH without chromatographic separation is demonstrated via SFS. The non-destructive nature of SFS provides ample opportunity for further metabolite confirmation via chromatographic techniques.
Show less - Date Issued
- 2013
- Identifier
- CFE0005102, ucf:50761
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005102
- Title
- Assessment of molecular interactions via magnetic relaxation: a quest for inhibitors of the anthrax toxin.
- Creator
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Santiesteban, Oscar, Perez Figueroa, Jesus, Liao, Yi, Yestrebsky, Cherie, Hampton, Michael, Lambert, Stephen, University of Central Florida
- Abstract / Description
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Anthrax is severe disease caused by the gram-positive Bacillus anthracis that can affect humans with deadly consequences. The disease propagates via the release of bacterial spores that can be naturally found in animals or can be weaponized and intentionally released into the atmosphere in a terrorist attack. Once inhaled, the spores become activated and the anthrax bacterium starts to reproduce and damage healthy macrophages by the release of the anthrax toxin. The anthrax toxin is composed...
Show moreAnthrax is severe disease caused by the gram-positive Bacillus anthracis that can affect humans with deadly consequences. The disease propagates via the release of bacterial spores that can be naturally found in animals or can be weaponized and intentionally released into the atmosphere in a terrorist attack. Once inhaled, the spores become activated and the anthrax bacterium starts to reproduce and damage healthy macrophages by the release of the anthrax toxin. The anthrax toxin is composed of three virulent factors: (i) anthrax protective antigen (APA), (ii) anthrax lethal factor (ALF), and (iii) anthrax edema factor (AEF) that work in harmony to effectuate the lethality associated with the disease. Out of the two internalized factors, ALF has been identified to play a critical role in cell death. Studies in animals have shown that mice infected with an anthrax strain lacking ALF survive the infection whereas when ALF is present the survivability of the mice is eliminated. Although the current therapy for anthrax is antibiotic treatment, modern medicine faces some critical limitations when combating infections. Antibiotics have proven very efficient in eliminating the bacterial infection but they lack the ability to destroy or inhibit the toxins released by the bacteria. This is a significant problem since ALF can remain active in the body for days after the infection is eliminated with no way of inhibiting its destructive effects. The use of inhibitors of ALF is an attractive method to treat the pathogenesis of anthrax infections. Over the last decade several inhibitors of the enzymatic activity of ALF have been identified. In order to identify inhibitors of ALF a variety of screening approaches such as library screenings, Mass Spectroscopy- based screenings and scaffold-based NMR screening have been used. Results from these screening have yielded mainly small molecules that can inhibit ALF in low micromolar to nanomolar concentrations. Yet, although valuable, these results have very little significance with regards to treating ALF in a real-life scenario since pharmaceutical companies are not willing to invest in further developing these inhibitors. Furthermore, the low incidence of inhalation anthrax, the lack of a market for an ALF inhibitor, and the expenses associated with the approval process of the FDA, have hindered the motivation of pharmaceutical companies to pursuit these kind of drugs. Therefore we have screened a small-molecule library of FDA approved drugs and common molecules in order to identify currently approved FDA drugs that can also inhibit ALF (Chapter III). The screening revealed that five molecules: sulindac, fusaric acid, naproxen, ketoprofen and ibuprofen bound to either ALF or APA with sulindac binding both. Additionally, we have developed a nanoparticle-based screening method that assesses molecular interactions by magnetic relaxation changes (Chapter II). Using this assay, we were able to accurately measure the dissociation constants of different interactions between several ligands and macromolecules. Moreover, we have used computational docking studies to predict the binding site of the identified molecules on the ALF or APA (Chapter IV). These studies predicted that two molecules sulindac and fusaric acid could be potential inhibitors of ALF since they bind at the enzymatic pocket. As a result, we tested the inhibitory potential of these molecules as well as that of the metabolic derivatives of sulindac (Chapter V). Results from these studies provided conclusive evidence that fusaric acid and sulindac were both strong inhibitors of ALF. Furthermore, the metabolic derivatives of sulindac, sulindac sulfide and sulindac sulfone also inhibited ALF. Overall, taking together these results we have discovered the alternate use of a currently used drug for the treatment of ALF pathogenesis.
Show less - Date Issued
- 2012
- Identifier
- CFE0004794, ucf:49745
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004794
- Title
- Novel optical properties of metal nanostructures based on surface plasmons.
- Creator
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Wang, Haining, Zou, Shengli, Liao, Yi, Kolpashchikov, Dmitry, Gesquiere, Andre, Su, Ming, University of Central Florida
- Abstract / Description
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Surface plasmons have been attracted extensive interests in recent decades due to the novel properties in nanometer sized dimensions. My work focused on the novel optical properties of metal nanostructures based on surface plasmons using theoretical simulation methods. In the first part, we investigated metal nanofilms and nanorods and demonstrated that extremely low scattering efficiency, high absorption efficiency and propagation with long distance could be obtained by different metal...
Show moreSurface plasmons have been attracted extensive interests in recent decades due to the novel properties in nanometer sized dimensions. My work focused on the novel optical properties of metal nanostructures based on surface plasmons using theoretical simulation methods. In the first part, we investigated metal nanofilms and nanorods and demonstrated that extremely low scattering efficiency, high absorption efficiency and propagation with long distance could be obtained by different metal nanostructures. With a perforated silver film, we demonstrated that an extremely low scattering cross section with an efficiency of less than 1% can be achieved at tunable wavelengths with tunable widths. The resonance wavelength, width, and intensity are influenced by the shape, size and arrangement pattern of the holes, as well as the distance separating the holes along the polarization direction. The extremely low scattering could be used to obtain high absorption efficiency of a two-layer silver nanofilm. Using the discrete dipole approximation method, we achieved enhanced absorption efficiencies, which are close to 100%, at tunable wavelengths in a two-layer silver thin film. The film is composed of a 100 nm thick perforated layer facing the incident light and a 100 nm thick solid layer. Resonance wavelengths are determined by the distances between perforated holes in the first layer as well as the separation between two layers. The resonance wavelengths shift to red with increasing separation distance between two layers or the periodic distance of the hole arrays. Geometries of conical frustum shaped holes in the first layer are critical for the improved absorption efficiencies. When the hole bottom diameter equals the periodic distance and the upper diameter is about one-third of the bottom diameter, close to unit absorption efficiency can be obtained. We examined the electromagnetic wave propagation along a hollow silver nanorod with subwavelength dimensions. The calculations show that light may propagate along the hollow nanorod with growing intensities. The influences of the shape, dimension, and length of the rod on the resonance wavelength and the enhanced local electric field, |E|2, along the rod were investigated. In the second part, a generalized electrodynamics model is proposed to describe the enhancement and quenching of fluorescence signal of a dye molecule placed near a metal nanoparticle (NP). Both the size of the Au NPs and quantum yield of the dye molecule are crucial in determining the emission intensity of the molecule. Changing the size of the metal NP will alter the ratio of the scattering and absorption efficiencies of the metal NP and consequently result in different enhancement or quenching effect to the dye molecule. A dye molecule with a reduced quantum yield indicates that the non-radiative channel is dominant in the decay of the excited dye molecules and the amplification of the radiative decay rate will be easier. In general, the emission intensity will be quenched when the size of metal NP is small and the quantum yield of dye molecule is about unity. A significant enhancement factor will be obtained when the quantum yield of the molecule is small and the particle size is large. When the quantum yield of the dye molecule is less than 10-5, the model is simplified to the surface enhanced Raman scattering equation.
Show less - Date Issued
- 2013
- Identifier
- CFE0004769, ucf:49786
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004769
- Title
- Photophysical and photochemical factors affecting multi-photon direct laser writing using the cross-linkable epoxide SU-8.
- Creator
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Williams Jr., Henry, Kuebler, Stephen, Elsheimer, Seth, Zhai, Lei, Liao, Yi, Heinrich, Helge, University of Central Florida
- Abstract / Description
-
For the past decade, the epoxy based photoresist SU-8 has been used commercially and in the lab for fabricating micro- and nano-structures. Investigators have studied how processing parameters such as pre- and post-exposure bake temperatures affect the resolution and quality of SU-8 structures patterned using ultraviolet or x-ray lithography. Despite the advances in understanding the phenomena, not all of them have been explored, especially those that are specific to multi-photon direct laser...
Show moreFor the past decade, the epoxy based photoresist SU-8 has been used commercially and in the lab for fabricating micro- and nano-structures. Investigators have studied how processing parameters such as pre- and post-exposure bake temperatures affect the resolution and quality of SU-8 structures patterned using ultraviolet or x-ray lithography. Despite the advances in understanding the phenomena, not all of them have been explored, especially those that are specific to multi-photon direct laser writing (mpDLW). Unlike conventional exposure techniques, mpDLW is an inherently three-dimensional (3D) process that is activated by nonlinear absorption of light.This dissertation reports how several key processing parameters affect mpDLW using SU-8 including pre-exposure bake duration, focal depth, incident laser power, focal-point scan speed, and excitation wavelength. An examination of solvent content of films at various stages in the mpDLW by 1H-NMR shows that even moderate solvent content (over 1 wt-%) affects film viscosity and photoacid diffusion lengths, and can greatly affect the overall fidelity of small features. A study of micro-fabricated feature size versus writing depth in the material shows that even slight refractive index mismatch between SU-8 and the medium between it and the focusing objective introduces spherical aberration that distorts the focus, causing feature size to decrease or even increase in size with writing depth, depending on the average exposure power used. Proper adjustment of the average exposure power was demonstrated as a means to fabricate more uniform features with writing depth. Third, when varying the power and scan speed, it was observed that the feature-size scales with these two parameters in a manner that is consistent with a three-photon absorption mechanism at an excitation wavelength of 800 nm. When aniiiexcitation wavelength of 725 nm is used, the feature-size scaling becomes consistent with that of two photon absorption. This shows that the photoinitiators in the SU-8 can be activated by either two- or three-photon absorption over this wavelength range. Using an irradiance of ~2 TW cm-2 and elongated femtosecond pulses resulted in an observed fourth order power dependence. This observation is in agreement with the literature and suggests that the effective absorptive nonlinearity is also sensitive to pulse duration. These findings will be useful for creating accurate models of the process of mpDLW in SU-8. These models could be used to optimize the processing parameters and develop new processing methods and materials for high-resolution fabrication of robust 3D microstructures. Some of the findings were used to develop a method for fabricating functional microlenses on the tip of optical fibers. This approach opens a new route to functional integrated photonic devices.
Show less - Date Issued
- 2013
- Identifier
- CFE0005441, ucf:50403
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005441
- Title
- Synthesis and Properties of Self-Assembled C/SiCN Nanocomposite Derived from Polymer Precursors.
- Creator
-
Li, Cheng, An, Linan, Fang, Jiyu, Coffey, Kevin, Liao, Yi, Xu, Chengying, Zhai, Lei, University of Central Florida
- Abstract / Description
-
The properties of C/SiCN nanocomposites synthesized by thermal decomposition of polymer precursors were studied in this work. The novel polymer-to-ceramic process enables us to tailor the ceramic structure in atomic level by designing the starting chemicals and pyrolysis procedures. It is of both fundamental and practical significance to investigate the properties and structures relationship of the nanocomposites. In this work, we explored their application potential in using as anode of...
Show moreThe properties of C/SiCN nanocomposites synthesized by thermal decomposition of polymer precursors were studied in this work. The novel polymer-to-ceramic process enables us to tailor the ceramic structure in atomic level by designing the starting chemicals and pyrolysis procedures. It is of both fundamental and practical significance to investigate the properties and structures relationship of the nanocomposites. In this work, we explored their application potential in using as anode of lithium-ion secondary batteries. The structure and structural evolution of C/SiCN nanocomposite were investigated by using XRD, FTIR, SEM, TEM, Solid state NMR and Raman spectroscopy. The results revealed the nanocomposites consisted of amorphous SiCxNx-4 matrix and carbon nanoclusters distributed within it. The size of the carbon was measured by Raman spectroscopy, varied with starting chemicals and pyrolysis temperature. The electronic properties of the C/SiCN nanocomposite were studied by measuring the I-V curves and a.c. impedance. The d.c. conductivity increased with carbon content and pyrolysis temperatures. The impedance spectra and fitted equivalent circuit results confirmed the existence of two phases in the nanocomposite. The possibility of using C/SiCN as anode in lithium-ion secondary batteries was investigated by electrochemical measurements, namely cyclic voltammetry, galvanostatic cyclic test and electrochemical impedance spectroscopy. The galvanostatic measurements showed that the nanocomposite with 26% of carbon nanoclusters exhibited a specific capacity of 480 mAh/g, which is 30% higher than that of commercial graphite anode. The high capacity of the nanocomposites is attributed to the formation of a novel structure around C/SiCN interface. The excellent electrochemical properties, together with the simple, low-cost processing, make the nanocomposites very promising for Li-ion battery applications.
Show less - Date Issued
- 2012
- Identifier
- CFE0004194, ucf:49028
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004194
