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Description
Magnetic Resonance Imaging using spiral trajectories has many advantages in speed, efficiency in data-acquistion and robustness to motion and flow related artifacts. The increase in sampling speed, however, requires high performance of the gradient system. Hardware inaccuracies from system delays and eddy currents can cause spatial and temporal distortions in the encoding gradient waveforms. This causes sampling discrepancies between the actual and the ideal k-space trajectory. Reconstruction assuming an ideal trajectory can result in shading and blurring artifacts in spiral images. Current methods to estimate such hardware errors require many modifications to the pulse sequence, phantom measurements or specialized hardware. This work presents a new method to estimate time-varying system delays for spiral-based trajectories. It requires a minor modification of a conventional stack-of-spirals sequence and analyzes data collected on three orthogonal cylinders. The method is fast, robust to off-resonance effects, requires no phantom measurements or specialized hardware and estimate variable system delays for the three gradient channels over the data-sampling period. The initial results are presented for acquired phantom and in-vivo data, which show a substantial reduction in the artifacts and improvement in the image quality.
ContributorsBhavsar, Payal (Author) / Pipe, James G (Thesis advisor) / Frakes, David (Committee member) / Kodibagkar, Vikram (Committee member) / Arizona State University (Publisher)
Created2013
Description
Gold nanoparticles have emerged as promising nanomaterials for biosensing, imaging, photothermal treatment and therapeutic delivery for several diseases, including cancer. We have generated poly(amino ether)-functionalized gold nanorods (PAE-GNRs) using a layer-by-layer deposition approach. Sub-toxic concentrations of PAE-GNRs were employed to deliver plasmid DNA to prostate cancer cells in vitro. PAE-GNRs generated using 1,4C-1,4Bis, a cationic polymer from our laboratory demonstrated significantly higher transgene expression and exhibited lower cytotoxicities when compared to similar assemblies generated using 25 kDa poly(ethylene imine) (PEI25k-GNRs), a current standard for polymer-mediated gene delivery. Additionally, sub-toxic concentrations of 1,4C-1,4Bis-GNR nanoassemblies were employed to deliver expression vectors that express shRNA ('shRNA plasmid') against firefly luciferase gene in order to knock down expression of the protein constitutively expressed in prostate cancer cells. The roles of poly(amino ether) chemistry and zeta-potential in determining transgene expression efficacies of PAE-GNR assemblies were investigated. The theranostic potential of 1,4C-1,4Bis-GNR nanoassemblies was demonstrated using live cell two-photon induced luminescence bioimaging. The PAE class of polymers was also investigated for the one pot synthesis of both gold and silver nanoparticles using a small library poly(amino ethers) derived from linear-like polyamines. Efficient nanoparticle synthesis dependent on concentration of polymers as well as polymer chemical composition is demonstrated. Additionally, the application of poly(amino ether)-gold nanoparticles for transgene delivery is demonstrated in 22Rv1 and MB49 cancer cell lines. Base polymer, 1,4C-1,4Bis and 1,4C-1,4Bis templated and modified gold nanoparticles were compared for transgene delivery efficacies. Differences in morphology and physiochemical properties were investigated as they relate to differences in transgene delivery efficacy. There were found to be minimal differences suggestion that 1,4C-1,4Bis efficacy is not lost following use for nanoparticle modification. These results indicate that poly(amino ether)-gold nanoassemblies are a promising theranostic platform for delivery of therapeutic payloads capable of simultaneous gene silencing and bioimaging.
ContributorsRamos, James (Author) / Rege, Kaushal (Thesis advisor) / Kodibagkar, Vikram (Committee member) / Caplan, Michael (Committee member) / Vernon, Brent (Committee member) / Garcia, Antonio (Committee member) / Arizona State University (Publisher)
Created2014
Description
This research reports on the investigation into the synthesis and stabilization of
iron oxide nanoparticles for theranostic applications using amine-epoxide polymers. Although theranostic agents such as magnetic nanoparticles have been designed and developed for a few decades, there is still more work that needs to be done with the type of materials that can be used to stabilize or functionalize these particles if they are to be used for applications such as drug delivery, imaging and hyperthermia. For in-vivo applications, it is crucial that organic coatings enclose the nanoparticles in order to prevent aggregation and facilitate efficient removal from the body as well as protect the body from toxic material.
The objective of this thesis is to design polymer coated magnetite nanoparticles with polymers that are biocompatible and can stabilize the iron oxide nanoparticle to help create mono-dispersed particles in solution. It is desirable to also have these nanoparticles possess high magnetic susceptibility in response to an applied magnetic field. The co- precipitation method was selected because it is probably the simplest and most efficient chemical pathway to obtain magnetic nanoparticles.
In literature, cationic polymers such as Polyethylenimine (PEI), which is the industry standard, have been used to stabilize IONPs because they can be used in magnetofections to deliver DNA or RNA. PEI however is known to interact very strongly with proteins and is cytotoxic, so as mentioned previously the Iron Oxide nanoparticles
i
(IONPs) synthesized in this study were stabilized with amine-epoxide polymers because of the limitations of PEI.
Four different amine-epoxide polymers which have good water solubility, biodegradability and less toxic than PEI were synthesized and used in the synthesis and stabilization of the magnetic nanoparticles and compared to PEI templated IONPs. These polymer-templated magnetic nanoparticles were also characterized by size, surface charge, Iron oxide content (ICP analysis) and superconducting quantum interference devices (SQUID) analysis to determine the magnetization values. TEM images were also used to determine the shape and size of the nanoparticles. All this was done in an effort to choose two or three leads that could be used in future work for magnetofections or drug delivery research.
iron oxide nanoparticles for theranostic applications using amine-epoxide polymers. Although theranostic agents such as magnetic nanoparticles have been designed and developed for a few decades, there is still more work that needs to be done with the type of materials that can be used to stabilize or functionalize these particles if they are to be used for applications such as drug delivery, imaging and hyperthermia. For in-vivo applications, it is crucial that organic coatings enclose the nanoparticles in order to prevent aggregation and facilitate efficient removal from the body as well as protect the body from toxic material.
The objective of this thesis is to design polymer coated magnetite nanoparticles with polymers that are biocompatible and can stabilize the iron oxide nanoparticle to help create mono-dispersed particles in solution. It is desirable to also have these nanoparticles possess high magnetic susceptibility in response to an applied magnetic field. The co- precipitation method was selected because it is probably the simplest and most efficient chemical pathway to obtain magnetic nanoparticles.
In literature, cationic polymers such as Polyethylenimine (PEI), which is the industry standard, have been used to stabilize IONPs because they can be used in magnetofections to deliver DNA or RNA. PEI however is known to interact very strongly with proteins and is cytotoxic, so as mentioned previously the Iron Oxide nanoparticles
i
(IONPs) synthesized in this study were stabilized with amine-epoxide polymers because of the limitations of PEI.
Four different amine-epoxide polymers which have good water solubility, biodegradability and less toxic than PEI were synthesized and used in the synthesis and stabilization of the magnetic nanoparticles and compared to PEI templated IONPs. These polymer-templated magnetic nanoparticles were also characterized by size, surface charge, Iron oxide content (ICP analysis) and superconducting quantum interference devices (SQUID) analysis to determine the magnetization values. TEM images were also used to determine the shape and size of the nanoparticles. All this was done in an effort to choose two or three leads that could be used in future work for magnetofections or drug delivery research.
ContributorsTamakloe, Beatrice (Author) / Rege, Kaushal (Thesis advisor) / Kodibagkar, Vikram (Committee member) / Chang, John (Committee member) / Arizona State University (Publisher)
Created2014
Description
Environmentally responsive microgels have drawn significant attention due to their intrinsic ability to change volume in response to various external stimuli such as pH, temperature, osmotic pressure, or electric and magnetic fields. The extent of particle swelling is controlled by the nature of the polymer-solvent interaction. This thesis focuses on design and synthesis of environmentally responsive microgels and their composites, and encompasses methods of utilizing microgel systems in applications as vehicles for the adsorption, retention, and targeted delivery of chemical species. Furthermore, self-assembled microgel particles at ionic liquid (IL)-water interfaces demonstrate responsive colloidal lattice morphology. The thesis first reports on the fundamental aspects of synthesis, functionalization, and characteristic properties of multifunctional environmentally responsive microgels derived from poly(N-isopropylacrylamide) (PNIPAm) and other functional co-monomers. In particular, the uptake and release of active chemical species such as rheology modifiers into and from these ionic microgels is demonstrated. Moreover, a facile tunable method for the formation of organic-inorganic composites with Fe3O4 nanoparticles adsorbed and embedded within ionic microgel particles is explored. Additionally, the development of zwitterionic microgels (ZI-MG) is presented. These aqueous ZI-MG dispersions exhibit reversible parabolic swelling as a function of pH and display a minimum hydrodynamic diameter at a tunable isoelectric point (IEP). This study also elucidates the controlled uptake and release of surfactants from these particle systems. The extent of surfactant loading and the ensuing relative swelling/deswelling behaviors within the polymer networks are explained in terms of their binding interactions. The latter part of this thesis highlights the versatility of fluorescently labeled microgel particles as stabilizers for IL-water droplets. When the prepared particles form monolayers and equilibrate at the liquid-liquid interface, the colloidal lattice organization may re-order itself depending on the surface charge of these particles. Finally, it is shown that the spontaneously formed and densely packed layers of microgel particles can be employed for extraction applications, as the interface remains permeable to small active species.
ContributorsChen, Haobo (Author) / Dai, Lenore L (Committee member) / Chen, Kangping (Committee member) / Forzani, Erica (Committee member) / Lind, Mary Laura (Committee member) / Mu, Bin (Committee member) / Arizona State University (Publisher)
Created2015
Description
Membranes are a key part of pervaporation processes, which is generally a more
efficient process for selective removal of alcohol from water than distillation. It is
necessary that the membranes have high alcohol permeabilities and selectivities.
Polydimethylsiloxane (PDMS) based mixed matrix membranes (MMMs) have
demonstrated very promising results. Zeolitic imidazolate framework-71 (ZIF-71)
demonstrated promising alcohol separation abilities. In this dissertation, we present
fundamental studies on the synthesis of ZIF-71/PDMS MMMs.
Free-standing ZIF-71/ PDMS membranes with 0, 5, 25 and 40 wt % ZIF-71
loadings were prepared and the pervaporation separation for ethanol and 1-butanol from
water was measured. ZIF-71/PDMS MMMs were formed through addition cure and
condensation cure methods. Addition cure method was not compatible with ZIF-71
resulting in membranes with poor mechanical properties, while the condensation cure
method resulted in membranes with good mechanical properties. The 40 wt % ZIF-71
loading PDMS nanocomposite membranes achieved a maximum ethanol/water selectivity
of 0.81 ± 0.04 selectivity and maximum 1-butnaol/water selectivity of 5.64 ± 0.15.
The effects of synthesis time, temperature, and reactant ratio on ZIF-71 particle
size and the effect of particle size on membrane performance were studied. Temperature
had the greatest effect on ZIF-71 particle size as the synthesis temperature varied from -
20 to 35 ºC. The ZIF-71 synthesized had particle diameters ranging from 150 nm to 1
μm. ZIF-71 particle size is critical in ZIF-71/PDMS composite membrane performance
for alcohol removal from water through pervaporation. The membranes made with
micron sized ZIF-71 particles showed higher alcohol/water selectivity than those with
smaller particles. Both alcohol and water permeability increased when larger sized ZIF-
71 particles were incorporated.
ZIF-71 particles were modified with four ligands through solvent assisted linker
exchange (SALE) method: benzimidazole (BIM), 5-methylbenzimidazole (MBIM), 5,6-
dimethylbenzimidazole (DMBIM) and 4-Phenylimidazole (PI). The morphology of ZIF-
71 were maintained after the modification. ZIF-71/PDMS composite membranes with 25
wt% loading modified ZIF-71 particles were made for alcohol/water separation. Better
particle dispersion in PDMS polymer matrix was observed with the ligand modified ZIFs.
For both ethanol/water and 1-butanol/water separations, the alcohol permeability and
alcohol/water selectivity were lowered after the ZIF-71 ligand exchange reaction.
efficient process for selective removal of alcohol from water than distillation. It is
necessary that the membranes have high alcohol permeabilities and selectivities.
Polydimethylsiloxane (PDMS) based mixed matrix membranes (MMMs) have
demonstrated very promising results. Zeolitic imidazolate framework-71 (ZIF-71)
demonstrated promising alcohol separation abilities. In this dissertation, we present
fundamental studies on the synthesis of ZIF-71/PDMS MMMs.
Free-standing ZIF-71/ PDMS membranes with 0, 5, 25 and 40 wt % ZIF-71
loadings were prepared and the pervaporation separation for ethanol and 1-butanol from
water was measured. ZIF-71/PDMS MMMs were formed through addition cure and
condensation cure methods. Addition cure method was not compatible with ZIF-71
resulting in membranes with poor mechanical properties, while the condensation cure
method resulted in membranes with good mechanical properties. The 40 wt % ZIF-71
loading PDMS nanocomposite membranes achieved a maximum ethanol/water selectivity
of 0.81 ± 0.04 selectivity and maximum 1-butnaol/water selectivity of 5.64 ± 0.15.
The effects of synthesis time, temperature, and reactant ratio on ZIF-71 particle
size and the effect of particle size on membrane performance were studied. Temperature
had the greatest effect on ZIF-71 particle size as the synthesis temperature varied from -
20 to 35 ºC. The ZIF-71 synthesized had particle diameters ranging from 150 nm to 1
μm. ZIF-71 particle size is critical in ZIF-71/PDMS composite membrane performance
for alcohol removal from water through pervaporation. The membranes made with
micron sized ZIF-71 particles showed higher alcohol/water selectivity than those with
smaller particles. Both alcohol and water permeability increased when larger sized ZIF-
71 particles were incorporated.
ZIF-71 particles were modified with four ligands through solvent assisted linker
exchange (SALE) method: benzimidazole (BIM), 5-methylbenzimidazole (MBIM), 5,6-
dimethylbenzimidazole (DMBIM) and 4-Phenylimidazole (PI). The morphology of ZIF-
71 were maintained after the modification. ZIF-71/PDMS composite membranes with 25
wt% loading modified ZIF-71 particles were made for alcohol/water separation. Better
particle dispersion in PDMS polymer matrix was observed with the ligand modified ZIFs.
For both ethanol/water and 1-butanol/water separations, the alcohol permeability and
alcohol/water selectivity were lowered after the ZIF-71 ligand exchange reaction.
ContributorsYin, Huidan (Author) / Lind, Mary Laura (Thesis advisor) / Mu, Bin (Committee member) / Nielsen, David (Committee member) / Seo, Don (Committee member) / Lin, Jerry (Committee member) / Arizona State University (Publisher)
Created2017
Description
Nanoporous materials, with pore sizes less than one nanometer, have been incorporated as filler materials into state-of-the-art polyamide-based thin-film composite membranes to create thin-film nanocomposite (TFN) membranes for reverse osmosis (RO) desalination. However, these TFN membranes have inconsistent changes in desalination performance as a result of filler incorporation. The nano-sized filler’s transport role for enhancing water permeability is unknown: specifically, there is debate around the individual transport contributions of the polymer, nanoporous particle, and polymer/particle interface. Limited studies exist on the pressure-driven water transport mechanism through nanoporous single-crystal nanoparticles. An understanding of the nanoporous particles water transport role in TFN membranes will provide a better physical insight on the improvement of desalination membranes.
This dissertation investigates water permeation through single-crystal molecular sieve zeolite A particles in TFN membranes in four steps. First, the meta-analysis of nanoporous materials (e.g., zeolites, MOFs, and graphene-based materials) in TFN membranes demonstrated non-uniform water-salt permselectivity performance changes with nanoporous fillers. Second, a systematic study was performed investigating different sizes of non-porous (pore-closed) and nanoporous (pore-opened) zeolite particles incorporated into conventionally polymerized TFN membranes; however, the challenges of particle aggregation, non-uniform particle dispersion, and possible particle leaching from the membranes limit analysis. Third, to limit aggregation and improve dispersion on the membrane, a TFN-model membrane synthesis recipe was developed that immobilized the nanoparticles onto the support membranes surface before the polymerization reaction. Fourth, to quantify the possible water transport pathways in these membranes, two different resistance models were employed.
The experimental results show that both TFN and TFN-model membranes with pore-opened particles have higher water permeance compared to those with pore-closed particles. Further analysis using the resistance in parallel and hybrid models yields that water permeability through the zeolite pores is smaller than that of the particle/polymer interface and higher than the water permeability of the pure polymer. Thus, nanoporous particles increase water permeability in TFN membranes primarily through increased water transport at particle/polymer interface. Because solute rejection is not significantly altered in our TFN and TFN-model systems, the results reveal that local changes in the polymer region at the polymer/particle interface yield high water permeability.
This dissertation investigates water permeation through single-crystal molecular sieve zeolite A particles in TFN membranes in four steps. First, the meta-analysis of nanoporous materials (e.g., zeolites, MOFs, and graphene-based materials) in TFN membranes demonstrated non-uniform water-salt permselectivity performance changes with nanoporous fillers. Second, a systematic study was performed investigating different sizes of non-porous (pore-closed) and nanoporous (pore-opened) zeolite particles incorporated into conventionally polymerized TFN membranes; however, the challenges of particle aggregation, non-uniform particle dispersion, and possible particle leaching from the membranes limit analysis. Third, to limit aggregation and improve dispersion on the membrane, a TFN-model membrane synthesis recipe was developed that immobilized the nanoparticles onto the support membranes surface before the polymerization reaction. Fourth, to quantify the possible water transport pathways in these membranes, two different resistance models were employed.
The experimental results show that both TFN and TFN-model membranes with pore-opened particles have higher water permeance compared to those with pore-closed particles. Further analysis using the resistance in parallel and hybrid models yields that water permeability through the zeolite pores is smaller than that of the particle/polymer interface and higher than the water permeability of the pure polymer. Thus, nanoporous particles increase water permeability in TFN membranes primarily through increased water transport at particle/polymer interface. Because solute rejection is not significantly altered in our TFN and TFN-model systems, the results reveal that local changes in the polymer region at the polymer/particle interface yield high water permeability.
ContributorsCay Durgun, Pinar (Author) / Lind, Mary Laura (Thesis advisor) / Lin, Jerry Y. S. (Committee member) / Green, Matthew D. (Committee member) / Seo, Dong K. (Committee member) / Tongay, Sefaattin (Committee member) / Arizona State University (Publisher)
Created2018
Description
The main objective of this research is to develop and characterize a targeted contrast agent that will recognize acute neural injury pathology (i.e. fibrin) after traumatic brain injury (TBI). Single chain fragment variable antibodies (scFv) that bind specifically to fibrin have been produced and purified. DSPE-PEG micelles have been produced and the scFv has been conjugated to the surface of the micelles; this nanoparticle system will be used to overcome limitations in diagnosing TBI. The binding and imaging properties will be analyzed in the future to determine functionality of the nanoparticle system in vivo.
ContributorsRumbo, Kailey Michelle (Author) / Stabenfeldt, Sarah (Thesis director) / Kodibagkar, Vikram (Committee member) / Barrett, The Honors College (Contributor) / Harrington Bioengineering Program (Contributor)
Created2014-05
Description
Smart contrast agents allow for noninvasive study of specific events or tissue conditions inside of a patient's body using Magnetic Resonance Imaging (MRI). This research aims to develop and characterize novel smart contrast agents for MRI that respond to temperature changes in tissue microenvironments. Transmission Electron Microscopy, Nuclear Magnetic Resonance, and cell culture growth assays were used to characterize the physical, magnetic, and cytotoxic properties of candidate nanoprobes. The nanoprobes displayed thermosensitve MR properties with decreasing relaxivity with temperature. Future work will be focused on generating and characterizing photo-active analogues of the nanoprobes that could be used for both treatment of tissues and assessment of therapy.
ContributorsHussain, Khateeb Hyder (Author) / Kodibagkar, Vikram (Thesis director) / Stabenfeldt, Sarah (Committee member) / Barrett, The Honors College (Contributor) / Harrington Bioengineering Program (Contributor) / School of Mathematical and Statistical Sciences (Contributor)
Created2014-05
Description
The overall goal of this project is to use metallic nanoparticles to develop a thin, ductile amorphous film at room temperature. Currently bulk metallic glasses are mainly formed via quenching, which requires very high cooling rates to achieve an amorphous molecular structure. These formations often fail in a brittle manner. The advantages of using a bottom-up approach with amorphous nanoparticles at ambient conditions is that the ductility of the metal can be improved, and the process will be less energy intensive. The nanoparticles used are iron precursors with ATMP and DTPMP ligand stabilizers and dispersed in methanol. Three forms of experimentation were applied over the course of this project. The first was a simple, preliminary data collection approach where the particles were dispersed onto a glass slide and left to dry under various conditions. The second method was hypersonic particle deposition, which accelerated the particles to high speeds and bombarded onto a glass or silicon substrate. The third method used Langmuir-Blodgett concepts and equipment to make a film. Qualitative analyses were used to determine the efficacy of each approach, including SEM imaging. In the end, none of the approaches proved successful. The first approach showed inconsistencies in the film formation and aggregation of the particles. The results from the hypersonic particle deposition technique showed that not enough particles were deposited to make a consistent film, and many of the particles that were able to be deposited were aggregated. The Langmuir-Blodgett method showed potential, but aggregation of the particles and uneven film formation were challenges here as well. Although there are ways the three discussed experimental approaches could be optimized, the next best step is to try completely new approaches, such as convective assembly and 3D printing to form the ideal nanoparticle film.
ContributorsKline, Katelyn Ann (Author) / Lind, Mary Laura (Thesis director) / Cay, Pinar (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-12
Description
Ionizing radiation, such as gamma rays and X-rays, are becoming more widely used. These high-energy forms of electromagnetic radiation are present in nuclear energy, astrophysics, and the medical field. As more and more people have the opportunity to be exposed to ionizing radiation, the necessity for coming up with simple and quick methods of radiation detection is increasing. In this work, two systems were explored for their ability to simply detect ionizing radiation. Gold nanoparticles were formed via radiolysis of water in the presence of Elastin-like polypeptides (ELPs) and also in the presence of cationic polymers. Gold nanoparticle formation is an indicator of the presence of radiation. The system with ELP was split into two subsystems: those samples including isopropyl alcohol (IPA) and acetone, and those without IPA and acetone. The samples were exposed to certain radiation doses and gold nanoparticles were formed. Gold nanoparticle formation was deemed to have occurred when the sample changed color from light yellow to a red or purple color. Nanoparticle formation was also checked by absorbance measurements. In the cationic polymer system, gold nanoparticles were also formed after exposing the experimental system to certain radiation doses. Unique to the polymer system was the ability of some of the cationic polymers to form gold nanoparticles without the samples being irradiated. Future work to be done on this project is further characterization of the gold nanoparticles formed by both systems.
ContributorsWalker, Candace (Author) / Rege, Kaushal (Thesis advisor) / Chang, John (Committee member) / Kodibagkar, Vikram (Committee member) / Potta, Thrimoorthy (Committee member) / Arizona State University (Publisher)
Created2012