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1.
Flack, Kyle M.
Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents.
Degree: PhD, Chemistry and Biochemistry, 2012, Georgia Tech
URL: http://hdl.handle.net/1853/44802 
► Green chemistry principles have been applied to the enhancement of two industrial chemistry problems. An industrially used reaction to form alcohols from aldehydes and ketones,…
(more)
▼ Green chemistry principles have been applied to the enhancement of two industrial chemistry problems. An industrially used reaction to form alcohols from aldehydes and ketones, the Meerwein-Ponndorf-Verley reduction, was improved by introducing a new catalyst Al(OtBu)₃. Due to the lower state of aggregation of this catalyst versus the conventional Al(OiPr)₃ catalyst, reduction rates were found to be faster in both pure iPrOH and mixed solvent systems for three model compounds: benzaldehyde, acetophenone, and a complex, chiral ketone, (S)-CMK. This allowed for the successful implementation of two important milestones; lowering the amount of catalyst needed necessary to complete the reactions (an economic benefit and lower waste) and the conversion from traditional batch reactions to continuous flow (a processing benefit) whereby reactions can be scaled-out rather than scaled-up. Another industrially important field of research that was focused on was CO₂ capture. High energy demands from current CO₂ capture methods such as aqueous amine solvents, specifically from coal-fired power plant flue gas, led to the development of non-aqueous reversible ionic liquids based on silylated amines. Structural modifications of the substitution around the silicon atom, the length of the alkyl chain bonding the silicon and amine, branching along the alkyl backbone, and investigating secondary and primary amines within this class of silylated amines were completed. These amines were reacted with CO₂ and the CO₂ capacity, the ionic liquid viscosity, reversal temperature and reaction enthalpy were all considered as a function of structure. In all cases the capacity was found to be not only greater than that of monethanolamine, an industrial standard, but higher than theoretical predictions through the formation of carbamic acid. Viscosity, reversal temperature, and reaction enthalpy were all found to be tunable through structure. These modifications gave significant insight into the necessary direction for optimization of these solvents as energy-efficient replacements of current CO₂ capture technology.
Advisors/Committee Members: Dr. Charles L. Liotta (Committee Chair), Dr. Charles A. Eckert (Committee Co-Chair), Dr. Angelo Bongiorno (Committee Member), Dr. Christopher Jones (Committee Member), Dr. Stefan France (Committee Member).
Subjects/Keywords: Silylated amines; Continuous flow; MPV reduction; Reversible ionic liquids; Carbon capture; Environmental chemistry Industrial applications; Carbon sequestration; Chemistry, Organic
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APA (6th Edition):
Flack, K. M. (2012). Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/44802
Chicago Manual of Style (16th Edition):
Flack, Kyle M. “Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents.” 2012. Doctoral Dissertation, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/44802.
MLA Handbook (7th Edition):
Flack, Kyle M. “Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents.” 2012. Web. 20 Jan 2021.
Vancouver:
Flack KM. Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents. [Internet] [Doctoral dissertation]. Georgia Tech; 2012. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/44802.
Council of Science Editors:
Flack KM. Two approaches to green chemistry in industrially driven processes: aluminum tert-butoxide as a rate enhancing Meerwein-Ponndorf-Verley reduction catalyst applied to the technological transfer from batch to continuous flow and structural modifications of functionalized trialkylsilylamines as energy efficient carbon dioxide capture solvents. [Doctoral Dissertation]. Georgia Tech; 2012. Available from: http://hdl.handle.net/1853/44802
2.
Hoskins, Travis Justin Christopher.
Carbon-carbon bond forming reactions
of biomass derived aldehydes.
Degree: MS, Chemical Engineering, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/29769
► The Knoevenagel reaction was applied to form a carbon-carbon double bond between the aldehydes (HMF, furfual) and an alpha di-carbonyl compound. The alpha di-carbonyl compound…
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▼ The Knoevenagel reaction was applied to form a carbon-carbon double bond between the aldehydes (HMF, furfual) and an alpha di-carbonyl compound. The alpha di-carbonyl compound used was malonic acid, which can be bio-derived from glucose along fermentation routes. The effects of solvents (THF, water, ethanol, isopropanol, ethyl ether, toluene) and catalysts (e.g. homogeneous and heterogeneous amines, solid basic oxides) on the yields of alpha-beta unsaturated acids were investigated. It was found that the homogeneous amines worked well in THF solvent (90-100% conversion, 99% selectivity for furfural and HMF), while the poly(styrene) supported ethylenediamine gave a higher conversion and selectivity for HMF (65± 5%, 99% selectivity) over furfural (58 ± 7%, 99% selectivity). This trend was also present in competition reactions where both HMF and furfural were reacted in the same vessel. á-â Unsaturated mono-acids for both HMF and furfural were identified as minor side products. However, levulinic acid did not work as well under the conditions studied. Lastly, among the solvents studied, several caused precipitation of the Knoevenagel products.
Advisors/Committee Members: Dr. Christopher Jones (Committee Chair), Dr. Pradeep Agrawal (Committee Co-Chair), Dr. Sujit Banerjee (Committee Member), Dr. Tom Fuller (Committee Member).
Subjects/Keywords: HMF; Furfural; Knoevenagel; Biomass; Aldehydes; Biomass energy; Chemical bonds
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APA (6th Edition):
Hoskins, T. J. C. (2008). Carbon-carbon bond forming reactions
of biomass derived aldehydes. (Masters Thesis). Georgia Tech. Retrieved from http://hdl.handle.net/1853/29769
Chicago Manual of Style (16th Edition):
Hoskins, Travis Justin Christopher. “Carbon-carbon bond forming reactions
of biomass derived aldehydes.” 2008. Masters Thesis, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/29769.
MLA Handbook (7th Edition):
Hoskins, Travis Justin Christopher. “Carbon-carbon bond forming reactions
of biomass derived aldehydes.” 2008. Web. 20 Jan 2021.
Vancouver:
Hoskins TJC. Carbon-carbon bond forming reactions
of biomass derived aldehydes. [Internet] [Masters thesis]. Georgia Tech; 2008. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/29769.
Council of Science Editors:
Hoskins TJC. Carbon-carbon bond forming reactions
of biomass derived aldehydes. [Masters Thesis]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/29769
Georgia Tech
3.
Heintz, Eva Liang-Huang.
Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles.
Degree: PhD, Chemistry and Biochemistry, 2004, Georgia Tech
URL: http://hdl.handle.net/1853/4944
► Surface Biological Modification and Cellular Interactions of Magnetic Spinel Nanoparticles Eva Liang-Huang Heintz 191 Pages Directed by Dr. Z. John Zhang The interest in magnetic…
(more)
▼ Surface Biological Modification and Cellular Interactions of Magnetic Spinel Nanoparticles
Eva Liang-Huang Heintz
191 Pages
Directed by
Dr. Z. John Zhang
The interest in magnetic nanoparticles is multi-dimensional. Fundamentally, it is important to be able to control their magnetic properties and to correlate to specific applications. In biology, magnetic nanoparticles offer promising potential as magnetic carriers or chaperones for magnetic localization and manipulation of therapeutic reagents.
The synthesis of superparamagnetic CoFe2-xSmxO4 nanoparticles and the tunability of their magnetic properties by size and composition variations are discussed. An increase in size of CoSm0.19Fe1.81O4 nanoparticles produced an increase in blocking temperature and saturation magnetization, but a non-linear coercitivity response was observed with change in size. By varying the composition, the saturation magnetization of CoFe2-xSmxO4 decreased dramatically while the coercitivity increased when compared to native cobalt spinel ferrite (CoFe2O4) nanoparticles. These results demonstrate how the magnetic properties of cobalt spinel ferrite nanoparticles can be tailored to specific applications.
Surface modifications of cobalt spinel ferrite nanoparticles facilitated the conjugation of oligonucleotides. Using a transfection reagent, CoFe2O4 ??igonucleotide conjugates were delivered into mammalian cells. Post transfection, synchronized movement of cells in response to an external magnetic field was observed. This demonstrated the possibility of magnetic manipulation and localization of therapeutic reagents coupled to CoFe2O4 magnetic nanoparticles.
Results from this thesis demonstrate the potential role of magnetic spinel nanoparticles in cell biology and will facilitate the progress towards in vivo testing.
Advisors/Committee Members: Dr. Z. John Zhang (Committee Chair), Dr. Christopher Jones (Committee Member), Dr. Jiri Janata (Committee Member), Dr. L. Andrew Lyon (Committee Member), Dr. Laren Tolbert (Committee Member).
Subjects/Keywords: Magnetic nanoparticles; Spinel ferrite; Transfection; Magnetic manipulation; Samarium; Surface modification
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APA (6th Edition):
Heintz, E. L. (2004). Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/4944
Chicago Manual of Style (16th Edition):
Heintz, Eva Liang-Huang. “Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles.” 2004. Doctoral Dissertation, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/4944.
MLA Handbook (7th Edition):
Heintz, Eva Liang-Huang. “Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles.” 2004. Web. 20 Jan 2021.
Vancouver:
Heintz EL. Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles. [Internet] [Doctoral dissertation]. Georgia Tech; 2004. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/4944.
Council of Science Editors:
Heintz EL. Surface Biological Modification and Cellular Interactions of Magnetic Spinel Ferrite Nanoparticles. [Doctoral Dissertation]. Georgia Tech; 2004. Available from: http://hdl.handle.net/1853/4944
Georgia Tech
4.
Chafin, Raymond William, II.
Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification.
Degree: PhD, Chemical Engineering, 2007, Georgia Tech
URL: http://hdl.handle.net/1853/14562
► Organic/inorganic materials have a high potential to enable major advances in membrane performance. It has previously been impossible to develop polymeric systems with adequate transport…
(more)
▼ Organic/inorganic materials have a high potential to enable major advances in membrane performance. It has previously been impossible to develop polymeric systems with adequate transport properties for xylene purification. Zeolite membranes have been created with the appropriate selectivities; however low productivity, low mechanical durability, and high capital costs have kept these materials from being utilized. So-called mixed matrix hybrid organic/inorganic membranes combine the mechanical durability and cost effectiveness of polymeric membranes with the enhanced performance of zeolitic structures. This project will focus on investigating polymeric and molecular sieve materials for mixed matrix membrane use in xylene isomer separation as a model system. Torlon polyamide-imide has unique properties that should be potentially useful in a mixed matrix composite. Silicalite will be investigated as the dispersed phased given its proven applicability with xylene isomers.
The overarching goal is to establish an approach for creation of mixed matrix materials that can be broadly applied to challenging organic separations. This project has three specific goals: (1) characterization of Torlons inherent properties, processing ability, and important transport potential, (2) characterization of zeolite matching properties and the effect of interfacial engineering on these properties, and (3) development of appropriate approaches to combine the sieve and polymer to obtain a hybrid material with properties that match theoretically predicted separation property enhancements relative to the neat polymer. High temperature pervaporation will be used to evaluate material transport properties, as this experimental setup closely mimics the high activity vapor streams found in many industrial xylene processes. The results of this research will be used to develop a protocol for development of future mixed matrix membranes that may be applied to a variety of organic liquid systems.
Advisors/Committee Members: Dr. William Koros (Committee Chair), Dr. Andrew Lyon (Committee Member), Dr. Carson Mereditch (Committee Member), Dr. Christopher Jones (Committee Member), Dr. Jeff Miller (Committee Member).
Subjects/Keywords: Xylene; Torlon; Pervaporation; Membranes; Organic liquid separation; Polyamideimide
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APA (6th Edition):
Chafin, Raymond William, I. (2007). Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/14562
Chicago Manual of Style (16th Edition):
Chafin, Raymond William, II. “Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification.” 2007. Doctoral Dissertation, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/14562.
MLA Handbook (7th Edition):
Chafin, Raymond William, II. “Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification.” 2007. Web. 20 Jan 2021.
Vancouver:
Chafin, Raymond William I. Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification. [Internet] [Doctoral dissertation]. Georgia Tech; 2007. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/14562.
Council of Science Editors:
Chafin, Raymond William I. Torlon® and Silicalite Mixed Matrix Membranes for Xylene Isomer Purification. [Doctoral Dissertation]. Georgia Tech; 2007. Available from: http://hdl.handle.net/1853/14562
Georgia Tech
5.
Shiels, Rebecca Anne.
Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals.
Degree: PhD, Chemical Engineering, 2008, Georgia Tech
URL: http://hdl.handle.net/1853/29629
► Catalysis is an important field of study in chemical engineering and chemistry due to its application in a vast number of chemical transformations. Traditionally, catalysts…
(more)
▼ Catalysis is an important field of study in chemical engineering and chemistry due to its application in a vast number of chemical transformations. Traditionally, catalysts have been developed as homogeneous molecular species or as heterogeneous insoluble materials. While homogeneous catalysts are typically very active and selective, they are difficult to recover. Conversely, heterogeneous catalysts are easy to recover and reuse, but they generally are less selective. To address these issues, the immobilization of homogeneous catalyst analogs onto solid supports has been a subject of research for the past few decades. Nonetheless, the effects of immobilization are still not completely predictable, and so continued effort is required to develop new immobilized catalysts as well as to develop a better understanding of how different parameters affect catalytic behavior.
This dissertation presents the synthesis, characterization, and evaluation of new immobilized catalysts for different applications. First, a solid base catalyst supported on silica was developed and studied in the synthesis of cyclic carbonates from epoxides and carbon dioxide. Next, polymer and silica supported vanadium Schiff base catalysts were developed and evaluated for use in the oxidative kinetic resolution of alpha-hydroxy esters, an enantioselective reaction. Lastly, salen catalyst analogs with amine reactive functional groups were synthesized and characterized for grafting onto aminosilicas with different degrees of amine group isolation. The grafted catalysts were then tested to determine how catalyst spacing on the surface affects their behavior. Throughout the presentation of these results, comparisons are made amongst the new supported catalysts and relevant existing catalysts to discern general trends which could be applied to a wider range of immobilized catalysts. Finally, research opportunities for further improvements in these areas are suggested.
Advisors/Committee Members: Dr. Christopher Jones (Committee Chair), Dr. Dennis Hess (Committee Member), Dr. Hang Lu (Committee Member), Dr. Marcus Weck (Committee Member), Dr. Pradeep Agrawal (Committee Member).
Subjects/Keywords: Immobilized catalyst; Hydrolytic kinetic resolution; Vanadium; Oxidative kinetic resolution; Cyclic carbonate; SBA-15; Salen; Silica; Catalysts; Catalysis; Schiff bases
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APA (6th Edition):
Shiels, R. A. (2008). Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/29629
Chicago Manual of Style (16th Edition):
Shiels, Rebecca Anne. “Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals.” 2008. Doctoral Dissertation, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/29629.
MLA Handbook (7th Edition):
Shiels, Rebecca Anne. “Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals.” 2008. Web. 20 Jan 2021.
Vancouver:
Shiels RA. Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals. [Internet] [Doctoral dissertation]. Georgia Tech; 2008. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/29629.
Council of Science Editors:
Shiels RA. Synthesis, characterization, and evaluation of silica and polymer supported catalysts for the production of fine chemicals. [Doctoral Dissertation]. Georgia Tech; 2008. Available from: http://hdl.handle.net/1853/29629
Georgia Tech
6.
Bhandari, Dhaval Ajit.
Hollow fiber sorbents for the desulfurization of pipeline natural gas.
Degree: PhD, Chemical Engineering, 2010, Georgia Tech
URL: http://hdl.handle.net/1853/42838
► Pipeline natural gas is the primary fuel of choice for distributed fuel cell-based applications. The concentration of sulfur in odorized natural gas is about 30…
(more)
▼ Pipeline natural gas is the primary fuel of choice for distributed fuel cell-based applications. The concentration of sulfur in odorized natural gas is about 30 ppm, with acceptable levels being <1 ppm for catalyst stability in such applications. Packed bed technology for desulfurization suffers from several disadvantages including high pressure drop and slow regeneration rates that require large unit sizes.
We describe a novel Rapid Temperature Swing Adsorption (RTSA) system utilizing hollow fibers with polymer 'binder', impregnated with high loadings of sulfur selective sorbent 'fillers'. Steam and cooling water can be utilized to thermally swing the sorbent during the regeneration cycles. An impermeable, thin polymer barrier layer on the outside of fiber sorbents allows only thermal interactions with the regeneration media, thereby promoting consistent sorption capacity over repeated cycles. A simplified flow pattern minimizes pressure drop, porous core morphology maximizes sorption efficiencies, while small fiber dimensions allows for rapid thermal cycles.
Advisors/Committee Members: Dr. William J. Koros (Committee Chair), Dr. Christopher Jones (Committee Member), Dr. James Stevens (Committee Member), Dr. Pradeep Agrawal (Committee Member), Dr. Ronald Rousseau (Committee Member), Dr. Satish Kumar (Committee Member).
Subjects/Keywords: Membranes; Natural gas; Separations; Porous media; Zeolites; Desulfurization; Adsorbents; Sorbents; Adsorption; Separation (Technology); Porous materials
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APA (6th Edition):
Bhandari, D. A. (2010). Hollow fiber sorbents for the desulfurization of pipeline natural gas. (Doctoral Dissertation). Georgia Tech. Retrieved from http://hdl.handle.net/1853/42838
Chicago Manual of Style (16th Edition):
Bhandari, Dhaval Ajit. “Hollow fiber sorbents for the desulfurization of pipeline natural gas.” 2010. Doctoral Dissertation, Georgia Tech. Accessed January 20, 2021.
http://hdl.handle.net/1853/42838.
MLA Handbook (7th Edition):
Bhandari, Dhaval Ajit. “Hollow fiber sorbents for the desulfurization of pipeline natural gas.” 2010. Web. 20 Jan 2021.
Vancouver:
Bhandari DA. Hollow fiber sorbents for the desulfurization of pipeline natural gas. [Internet] [Doctoral dissertation]. Georgia Tech; 2010. [cited 2021 Jan 20].
Available from: http://hdl.handle.net/1853/42838.
Council of Science Editors:
Bhandari DA. Hollow fiber sorbents for the desulfurization of pipeline natural gas. [Doctoral Dissertation]. Georgia Tech; 2010. Available from: http://hdl.handle.net/1853/42838
. 
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