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Texas A&M University
1.
Sun, Rui.
Polymerized Ionic Liquid Derived Carbon.
Degree: MS, Chemical Engineering, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/157830
► The development of new carbon-based materials with exquisite control over surface chemistry, carbon structure and form, surface area, pore size, and conductivity is of significant…
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▼ The development of new carbon-based materials with exquisite control over surface chemistry, carbon structure and form, surface area, pore size, and conductivity is of significant interest for numerous applications, including energy storage (e.g., capacitors). Recently, a few studies have demonstrated the ability to produce carbon from ionic liquids (ILs) and polymerized ionic liquids (PILs), both of which have unique physiochemical properties and result in carbon with various surface chemistries depending on the chemistry of the IL or PIL. However, to date, few studies have explored the relationship between the possible diverse PIL chemistries and the resulting PIL-derived carbon properties. In this study, numerous PILs with various backbone/cation pairings (backbones: ethyl methacrylate, styrene; covalently attached cations: butylimidazolium, trimethylammonium, piperidinium, butylpyrrolidinium, methylpyrrolidinium) were synthesized as carbon precursors. The chemistry and molecular weight of the PILs were characterized using proton nuclear magnetic resonance (
1H NMR) spectroscopy, elemental analysis (EA), and gel permeation chromatography (GPC). PIL-derived carbons were produced from this set of PILs via pyrolysis at 10 °C/min. The surface chemistry, carbon structure and form, porosity, and conductivity of these PIL-derived carbons were characterized using X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). A fundamental investigation into the relationship between PIL chemistry and PIL-derived carbon properties was explored, along with the subsequent implications on electrode materials for energy storage applications.
Advisors/Committee Members: Elabd, Yossef A (advisor), Lutkenhaus, Jodie L (committee member), Fang, Lei (committee member).
Subjects/Keywords: Nitrogen-doped carbon; polymerized ionic liquids
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APA (6th Edition):
Sun, R. (2016). Polymerized Ionic Liquid Derived Carbon. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/157830
Chicago Manual of Style (16th Edition):
Sun, Rui. “Polymerized Ionic Liquid Derived Carbon.” 2016. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/157830.
MLA Handbook (7th Edition):
Sun, Rui. “Polymerized Ionic Liquid Derived Carbon.” 2016. Web. 21 Apr 2021.
Vancouver:
Sun R. Polymerized Ionic Liquid Derived Carbon. [Internet] [Masters thesis]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/157830.
Council of Science Editors:
Sun R. Polymerized Ionic Liquid Derived Carbon. [Masters Thesis]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/157830

Texas A&M University
2.
Kwon, Se Ra.
Organic Electrodes for Structural Energy and Power.
Degree: PhD, Chemical Engineering, 2017, Texas A&M University
URL: http://hdl.handle.net/1969.1/161490
► Structural power systems, which simultaneously provide structural and electrochemical energy storage functionalities, have arisen as an emerging need for a wide range of applications. A…
(more)
▼ Structural power systems, which simultaneously provide structural and electrochemical energy storage functionalities, have arisen as an emerging need for a wide range of applications. A challenge is to develop the multifunctional composite electrodes which can perform the acceptable energy storage and mechanical roles in a single platform. Composite electrodes containing graphene and polymers are designed using different processing techniques and examined in the context of multifunctional structural electrodes. The relationship between materials properties, processing methods, and performance of the composite electrodes is investigated.
Polyaniline nanofibers (PANI NF)/reduced graphene oxide (RGO) composite electrodes are fabricated using spray-assisted layer-by-layer (LbL) assembly. In this spray-on approach, the most critical parameters to create uniform electrodes are blow-drying time and removal of rinsing step. The architecture and electrochemical performance are investigated and compared against control electrodes made by dip-assisted LbL assembly. The spray-assisted PANI NF/RGO LbL electrodes exhibit over 70 times faster film growth behavior and a more porous structure than dip-assisted LbL electrodes. The increased porosity enables an enhanced rate capability and a higher power at a given specific energy compared to dip-assisted LbL electrodes.
To design multifunctional structural electrodes, mechanically strong aramid nanofibers (ANFs) are utilized as reinforcing building blocks and blended with graphene using different film fabrication techniques. RGO/ANF LbL films are fabricated using dip-assisted LbL assembly. The resulting electrodes exhibit an ANF-rich structure where ANFs act as a polymer matrix that interfacially interacts with RGO sheets. Chemical reduction leads to higher electrochemical performance. Nanomechanical testing shows that the electrodes have a modulus intermediate between the individual ANF and GO components. No cracks or defects are observed upon flexing 1000 times, which demonstrates that RGO/ANF LbL electrodes are promising for flexible, mechanically robust energy and power.
Free-standing RGO/ANF supercapacitor electrodes are fabricated via vacuum-assisted filtration and exhibit extraordinary mechanical strength and excellent electrochemical performance, which is attributed to the incorporation of ANFs as reinforcing nanofillers into the system where RGO sheets are interconnected with ANFs by non-covalent interfacial interactions. The RGO/ANF composite electrodes show multifunctionality superior to that of other graphene-based supercapacitors, indicating an excellent combination of both mechanical and electrochemical properties.
Advisors/Committee Members: Lutkenhaus, Jodie L. (advisor), Balbuena, Perla (committee member), Akbulut, Mustafa (committee member), Mukherjee, Partha (committee member).
Subjects/Keywords: Composite electrodes; Structural energy and power
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APA (6th Edition):
Kwon, S. R. (2017). Organic Electrodes for Structural Energy and Power. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/161490
Chicago Manual of Style (16th Edition):
Kwon, Se Ra. “Organic Electrodes for Structural Energy and Power.” 2017. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/161490.
MLA Handbook (7th Edition):
Kwon, Se Ra. “Organic Electrodes for Structural Energy and Power.” 2017. Web. 21 Apr 2021.
Vancouver:
Kwon SR. Organic Electrodes for Structural Energy and Power. [Internet] [Doctoral dissertation]. Texas A&M University; 2017. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/161490.
Council of Science Editors:
Kwon SR. Organic Electrodes for Structural Energy and Power. [Doctoral Dissertation]. Texas A&M University; 2017. Available from: http://hdl.handle.net/1969.1/161490

Texas A&M University
3.
O'Neal, Joshua Taylor.
Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites.
Degree: PhD, Materials Science and Engineering, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/173420
► This thesis presents three investigations into the responsive physical and thermal properties of polyelectrolyte layer-by-layer assemblies. The first study focuses on hydrogen bonded, layer-by-layer assembled…
(more)
▼ This thesis presents three investigations into the responsive physical and thermal properties of polyelectrolyte layer-by-layer assemblies. The first study focuses on hydrogen bonded, layer-by-layer assembled films and nanocomposites Polyelectrolyte multilayers and layer-by-layer assemblies are susceptible to structural changes in response to changes in the post-assembly environment. The study demonstrates the first reported use of spray-assisted layer-by-layer assembly to produce hydrogen-bonding polymer nanocomposites of poly(ethylene oxide) (PEO) and poly(methacrylic acid) (PMAA) containing discrete regions of gold nanoparticles (AuNPs) vertically positioned throughout the film structure with no substantial aggregation. Elevating the environmental pH disrupts the hydrogen bonding network, resulting in release of the AuNPs, and the rate of release is shown to depend on the pH of the environment.
The second study deals with the swelling response of electrostatic layer-by-layer thin films to changes in ionic environment. The effects of a wide range of KBr concentrations (0 to 1.6
M) on the swelling and deswelling of LbL assemblies formed from poly(diallyldimethylammonium) polycation (PDADMA) and poly(styrenesulfonate) polyanion (PSS) in 0.5
M NaCl were investigated using quartz-crystal microbalance with dissipation (QCM-D) monitoring. The swelling behavior is compared with responses to KCl, NaBr, and NaCl at various concentrations. The results demonstrate anion type dominates swelling response, and that Br- ions have a much greater effect on the structure of as-prepared thin films than Cl- at ionic strengths above assembly conditions, likely due to the chaotropic nature of Br^-. Four response regimes are identified that delineate swelling due to electrostatic repulsion, slight contraction, swelling due to doping, and film destruction as ionic strength increases.
The third study focuses on the thermal response of electrostatic layer-by-layer assemblies of PDADMA and PSS to changes in hydration level and counterion type. Modulated differential scanning calorimetry (MDSC) is employed to quantify the influence of changing hydration level, ionic strength and type, as well as assembly conditions on the glass transition temperature (Tg) of free-standing PDADMA/PSS LbL films assembled in 0.5
M NaCl. The results indicate that assembly conditions and post-assembly hydration level are the primary factor in determining the Tg of PDADMA/PSS LbL films when hydration is limited to less than 35 wt%. Hydrating with KBr solutions resulted in no apparent effect on the Tg of the LbL films. Conversely, films assembled in NaCl and KBr at identical ionic strengths show a nearly 20°C difference in Tg, indicating a different internal structure of extrinsic and intrinsic ion pairing. Finally, PDADMA/PSS LbL films show remarkably similar Tg behavior to PDADMA/PSS complexes when hydrated to similar levels.
Advisors/Committee Members: Lutkenhaus, Jodie L (advisor), Grunlan, Jaime (committee member), Sukhishvili, Svetlana (committee member), Elabd, Yossef (committee member).
Subjects/Keywords: layer-by-layer assembly; responsive; nanocomposites; thin films; swelling; glass transition temperature; monovalent counterions
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
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APA (6th Edition):
O'Neal, J. T. (2018). Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/173420
Chicago Manual of Style (16th Edition):
O'Neal, Joshua Taylor. “Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/173420.
MLA Handbook (7th Edition):
O'Neal, Joshua Taylor. “Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites.” 2018. Web. 21 Apr 2021.
Vancouver:
O'Neal JT. Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/173420.
Council of Science Editors:
O'Neal JT. Layer-by-Layer Assembly of Responsive Polyelectrolyte Thin Films and Nanocomposites. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/173420

Texas A&M University
4.
Chen, Tzu Ling.
Hybrid-Capacitor with Polyaniline/Carbon Electrodes.
Degree: MS, Chemical Engineering, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/157982
► Hybrid-capacitors have the potential to synergistically combine the benefits of both electrochemical double layer capacitors (EDLCs) (longer cycle life) and pseudo-capacitors (higher capacitance). However, new…
(more)
▼ Hybrid-capacitors have the potential to synergistically combine the benefits of both electrochemical double layer capacitors (EDLCs) (longer cycle life) and pseudo-capacitors (higher capacitance). However, new processes that intimately combine the two primary materials from each capacitor (carbon and conductive polymer, respectively) within the electrodes in an ordered fashion on the nanoscale are needed to realize this potential. In this study, we report on a physical method (simultaneous electro-spinning/electro-spraying (E/E)) and a chemical method (in situ oxidative polymerization) for fabricating hybrid-capacitors with high surface area electrodes consisting of polyaniline (PANI) and carbon materials (referred to as E/E electrodes).
E/E produces a PANI/carbon nanofiber/particle network with fiber diameters in the range of 500 to 2000 nm. The hybrid-capacitor with E/E electrodes exhibits an excellent specific capacitance of 235 F g^-1 (vs. 138 F g^-1 for capacitor with state-of-the art hybrid electrodes) at a current density of 1 A g^-1. Moreover, the capacitor with E/E electrodes retains approximately 84 % capacitance after 1000 charge-discharge cycles (vs. 67 % for capacitor with state-of-the art hybrid electrodes). A post mortem electron microscopy study of the E/E electrodes provides a rationale for the improved cycling stability. These results demonstrate the feasibility of producing E/E electrodes and their promise as future materials in hybrid-capacitors.
Multiwall carbon nanotube (MWCNT)/PANI composites synthesized via in situ oxidative polymerization show improved electrochemical performance in a capacitor compared with pure MWCNTs due to the compact chemical bonding between MWCNT and PANI. Hybrid-capacitors with E/E MWCNT-PANI composite electrodes were also investigated and showed improved performance. Capacitor performance has a high correlation with morphology and polymer-carbon interface and connectivity and can be modified by fabrication and synthetic processes. A deep fundamental understanding of charge storage mechanisms in hybrid materials will guide the design of future polymercarbon electrodes for hybrid-capacitors.
Advisors/Committee Members: Elabd, Yossef A. (advisor), Lutkenhaus, Jodie L. (committee member), Grunlan, Jaime (committee member).
Subjects/Keywords: electrospinning; electrospraying; hybrid-capacitor; pseudo-capacitor; polyaniline
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APA ·
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MLA ·
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APA (6th Edition):
Chen, T. L. (2016). Hybrid-Capacitor with Polyaniline/Carbon Electrodes. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/157982
Chicago Manual of Style (16th Edition):
Chen, Tzu Ling. “Hybrid-Capacitor with Polyaniline/Carbon Electrodes.” 2016. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/157982.
MLA Handbook (7th Edition):
Chen, Tzu Ling. “Hybrid-Capacitor with Polyaniline/Carbon Electrodes.” 2016. Web. 21 Apr 2021.
Vancouver:
Chen TL. Hybrid-Capacitor with Polyaniline/Carbon Electrodes. [Internet] [Masters thesis]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/157982.
Council of Science Editors:
Chen TL. Hybrid-Capacitor with Polyaniline/Carbon Electrodes. [Masters Thesis]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/157982

Texas A&M University
5.
Zhou, Jing.
Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery.
Degree: MS, Materials Science and Engineering, 2013, Texas A&M University
URL: http://hdl.handle.net/1969.1/151697
► Layer-by-layer (LbL) capsules, known for their versatility and smart response to environmental stimuli, have attracted great interest in drug delivery applications. However, achieving a desired…
(more)
▼ Layer-by-layer (LbL) capsules, known for their versatility and smart response to environmental stimuli, have attracted great interest in drug delivery applications. However, achieving a desired drug delivery system with sustained and tunable drug release in response to temperature is still challenging. Here, a thermo-responsive drug delivery system of solid dexamethasone nanoparticles (DXM NPs) encapsulated in a model LbL assembly of strong polyelectrolytes poly (diallyldimethylammonium chloride)/poly (styrene sulfonate) (PDAC/PSS) was constructed.
DXM NPs at an average size of 20196 nm were fabricated. ζ-potential measurements, X-ray photoelectron spectroscopy, and transmission electron microscopy confirmed the successful adsorption of each layer. The influence of various parameters on drug release, such as number of layers, ionic strength of the adsorption solution, temperature and outer-most layer, has been investigated. Results have shown a controlled DXM release from LbL nanoshells by tuning number of layers and ionic strength of the adsorption solution. The DXM release from linearly growing LbL of PDAC/PSS (assembled without NaCl), which do not exhibit a glass transition, experienced a more temperature response than those from exponentially growing LbL of PDAC/PSS (assembled at 0.5
M NaCl), which exhibit a glass transition. Such a difference was attributed to be related with the free volume cavities within the assemblies. By tailoring the properties of those cavities, an ideal thermo-responsive drug delivery system may be obtained. This thermo-responsive NP-based drug delivery system with tunable permeability may possibly realize an “on” or “off” drug release mechanism in response to temperature, thus providing an alternative approach to delivery therapeutics with reduced toxic effects.
Advisors/Committee Members: Pishko, Michael V. (advisor), Lutkenhaus, Jodie L. (advisor), Cheng, Zhengdong (committee member).
Subjects/Keywords: Thermo-Responsive; drug delivery
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APA ·
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MLA ·
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APA (6th Edition):
Zhou, J. (2013). Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/151697
Chicago Manual of Style (16th Edition):
Zhou, Jing. “Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery.” 2013. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/151697.
MLA Handbook (7th Edition):
Zhou, Jing. “Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery.” 2013. Web. 21 Apr 2021.
Vancouver:
Zhou J. Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery. [Internet] [Masters thesis]. Texas A&M University; 2013. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/151697.
Council of Science Editors:
Zhou J. Thermo-responsive Layer-by-Layer Assemblies for Nanoparticle-based Drug Delivery. [Masters Thesis]. Texas A&M University; 2013. Available from: http://hdl.handle.net/1969.1/151697

Texas A&M University
6.
Puhr, Joseph Timothy.
The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies.
Degree: MS, Materials Science and Engineering, 2014, Texas A&M University
URL: http://hdl.handle.net/1969.1/152854
► Nanoparticles can have a profound effect on a polymer’s glass transition temperature (T_(g)). Many layer-by-layer (LbL) assemblies contain nanoparticles for added functionality, but the resulting…
(more)
▼ Nanoparticles can have a profound effect on a polymer’s glass transition temperature (T_(g)). Many layer-by-layer (LbL) assemblies contain nanoparticles for added functionality, but the resulting effect of nanoparticles on an LbL film’s properties is not known. Previously, we have shown that a nanoparticle-free LbL film containing strong polyelectrolytes, poly(diallyldimethylammonium chloride)/poly(styrene sulfonate) (PDAC/PSS), exhibited a thermal transition somewhat akin to a glass transition using quartz crystal microblance with dissipation (QCM-D) and modulated differential
scanning calorimetry (MDSC). In the work presented here, layers of negatively charged nanoparticles of either spherical or platelet morphology have been inserted at varying locations throughout PDAC/PSS LbL films. QCM-D and MDSC were used to determine the effect that these nanoparticles have on the previously measured thermal transitions as a function of placement within the film and particle shape. Using QCM-D we observed clear, reproducible T_(g)’s in all LAP film configurations and in one particular SiO_(2) configuration. All observed T_(g)’s, regardless of nanoparticle morphology, were elevated with respect to those found in neat PDAC/PSS films. Additionally, there was little difference noted between the transition values for the two particular morphologies. It was discovered that the highest glass transition temperatures were observed for film
configurations where the nanoparticles were added during the middle bilayer. We attributed this phenomenon to the increased available nanoparticle surface area with which nearby polymer chains could form bonds. Unfortunately the extremely weak and broad thermal transitions observed with MDSC proved to be inconclusive in either supporting or refuting these observations made via QCM-D.
Advisors/Committee Members: Lutkenhaus, Jodie L (advisor), Grunlan, Jamie C (committee member), McShane, Michael J (committee member).
Subjects/Keywords: Glass Transition; Layer-by-Layer Assembly
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APA (6th Edition):
Puhr, J. T. (2014). The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/152854
Chicago Manual of Style (16th Edition):
Puhr, Joseph Timothy. “The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies.” 2014. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/152854.
MLA Handbook (7th Edition):
Puhr, Joseph Timothy. “The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies.” 2014. Web. 21 Apr 2021.
Vancouver:
Puhr JT. The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies. [Internet] [Masters thesis]. Texas A&M University; 2014. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/152854.
Council of Science Editors:
Puhr JT. The Effect of Nanoparticles on the Thermal Transitions of Hydrated Layer-by-Layer Assemblies. [Masters Thesis]. Texas A&M University; 2014. Available from: http://hdl.handle.net/1969.1/152854

Texas A&M University
7.
Kleiderer IV, Arthur Conrad.
Electrospun/Electrosprayed Aligned Fuel Cell Electrodes.
Degree: MS, Chemical Engineering, 2017, Texas A&M University
URL: http://hdl.handle.net/1969.1/165904
► Proton exchange membrane fuel cells (PEMFCs) are a promising technology in energy conversion. However, the high cost of the platinum catalyst limits the use of…
(more)
▼ Proton exchange membrane fuel cells (PEMFCs) are a promising technology in energy conversion. However, the high cost of the platinum catalyst limits the use of fuel cells. To address this problem, many improvements and optimizations have been proposed for the PEMFC catalyst layer. In this study, an apparatus to produce aligned Nafion fiber catalyst layers is designed, the alignment capabilities of the apparatus are explored, and the performance of the aligned catalyst layer is evaluated.
A horizontal accelerated drum is able to produce aligned Nafion fibers up to 80% alignment. This alignment is present at drum speeds over 3000 rpm over a wide range of electrospinning solution flow rates. A catalyst layer fabricated via simultaneous electrospinning and electrospraying (E/E) has a peak power density of 535 mW cmˉ² and an electrochemical surface area of 42 m² gˉ¹. This performance is comparable to the performance of a randomly aligned catalyst layer fabricated with E/E.
Advisors/Committee Members: Elabd, Yossef A. (advisor), Lutkenhaus, Jodie L. (committee member), Mukherjee, Partha (committee member).
Subjects/Keywords: fuel cell; catalyst layer; electrospinning; electrospraying; simultaneous; aligned
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APA (6th Edition):
Kleiderer IV, A. C. (2017). Electrospun/Electrosprayed Aligned Fuel Cell Electrodes. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/165904
Chicago Manual of Style (16th Edition):
Kleiderer IV, Arthur Conrad. “Electrospun/Electrosprayed Aligned Fuel Cell Electrodes.” 2017. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/165904.
MLA Handbook (7th Edition):
Kleiderer IV, Arthur Conrad. “Electrospun/Electrosprayed Aligned Fuel Cell Electrodes.” 2017. Web. 21 Apr 2021.
Vancouver:
Kleiderer IV AC. Electrospun/Electrosprayed Aligned Fuel Cell Electrodes. [Internet] [Masters thesis]. Texas A&M University; 2017. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/165904.
Council of Science Editors:
Kleiderer IV AC. Electrospun/Electrosprayed Aligned Fuel Cell Electrodes. [Masters Thesis]. Texas A&M University; 2017. Available from: http://hdl.handle.net/1969.1/165904

Texas A&M University
8.
Minaeian, Mahsa.
Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study.
Degree: MS, Chemistry, 2019, Texas A&M University
URL: http://hdl.handle.net/1969.1/188776
► Use of polymeric nanoparticles has gained significant interest in recent years for a wide spectrum of applications such as drug delivery, cell imaging, environmental remediation,…
(more)
▼ Use of polymeric nanoparticles has gained significant interest in recent years for a wide spectrum of applications such as drug delivery, cell imaging, environmental remediation, and, electronics. However, many of these nanoparticles have been mainly synthesized at the laboratory scale. Large scale synthesis of these nanoparticles in a cost-effective and reliable fashion could significantly expand their industrial use. In many cases, self-assembly of block polymers into different morphologies involves a transition from a solvated polymer in an organic solvent to a fully aqueous system. Here, the feasibility of using tangential flow filtration (TFF) to scale-up the solution-state transition was studied. A custom-designed and chemically resistant experimental TFF system was built. Nine TFF experiments were performed to study the effects of change of transmembrane pressure, nanoparticles concentration, and hydrophobic/hydrophilic block ratio on solvent removal and nanoparticle size evolution during the diafiltration process. In addition, three batch dialysis experiments were performed to understand the possible extent of scale-up using the proposed system.
The designed experimental setup had considerable chemical resistance to many solvents and could be used to conduct small-molecule removal, scaleup, and concentration processes on a wide range of polymers. Feasibility of use of TFF for purification of amphiphilic polymeric nanoparticles with core-shell morphology was demonstrated. Solvent exchange using TFF was considerably faster compared to the traditional batch dialysis system. In TFF experiments, the organic solvent concentration reached the minimum level after 1 hour of in-flow filtration, while it took around 6 hours to reach similar levels of solvent exchange in the batch setting. In addition to an order of magnitude higher processing volumes of TFF compared to dialysis, further scale-up of the TFF process is easily achievable with increasing the membrane area. As expected, higher transmembrane pressure resulted in faster organic solvent removal. The initial nanoparticles concentration had a significant effect on the diameter of the formed structures during the TFF purification, which affected the required purification time. A high ratio of hydrophobic to hydrophilic blocks in a block copolymer increases the chance of precipitation of nanoparticle during TFF, which might terminate the process.
Advisors/Committee Members: Wooley, Karen L. (advisor), Batteas, James D. (committee member), Lutkenhaus, Jodie L. (committee member).
Subjects/Keywords: scale-up; tangential flow filtration; polymeric nanoparticles purification; feasibility study
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APA ·
Chicago ·
MLA ·
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APA (6th Edition):
Minaeian, M. (2019). Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study. (Masters Thesis). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/188776
Chicago Manual of Style (16th Edition):
Minaeian, Mahsa. “Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study.” 2019. Masters Thesis, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/188776.
MLA Handbook (7th Edition):
Minaeian, Mahsa. “Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study.” 2019. Web. 21 Apr 2021.
Vancouver:
Minaeian M. Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study. [Internet] [Masters thesis]. Texas A&M University; 2019. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/188776.
Council of Science Editors:
Minaeian M. Scaled-up Purification of Poly(acrylic acid)-Block-Polystyrene Nanoparticles Using Tangential Flow Filtration: A Feasibility Study. [Masters Thesis]. Texas A&M University; 2019. Available from: http://hdl.handle.net/1969.1/188776

Texas A&M University
9.
Luo, Sheng.
Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media.
Degree: PhD, Petroleum Engineering, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/174434
► The phase behavior of petroleum fluids is an important factor in evaluating the hydrocarbon reserves and forecasting the oil and gas production behavior. Due to…
(more)
▼ The phase behavior of petroleum fluids is an important factor in evaluating the hydrocarbon reserves and forecasting the oil and gas production behavior. Due to the existence of nano-scale pores, the fluid phase behavior in unconventional shale reservoirs differs significantly from that in unconventional reservoirs. Practically, the complexities of phase behavior in shale is associated with several factors, such as confinement effect, pore size distribution, surface uncertainty and heterogeneous distribution of hydrocarbon species. Previous work has mostly focused on theoretical studies and simulations. However, there are relatively few experimental data to verify the theories and models. A comprehensive picture of pressure-volume-temperature (PVT) behavior for the confined hydrocarbons remains uncertain.
This study, combined with laboratory and simulation studies, is dedicated to understand fluid phase behavior under nano-confinement effect from both experimental and theoretical aspects. Firstly, we developed an experimental technique of differential scanning calorimetry to measure the hydrocarbon liquid-vapor phase transition temperature in nanopores. Next, the experimental data is used to correlate a pore-size-dependent equation of state (EOS). The confinement parameters in EOS are determined and the EOS is shown to predict experimental results. With the pore-size-dependent EOS, a multi-scale PVT simulator is developed for shale’s nano-scale pore size distribution systems. The PVT simulator realistically models the constant composition expansion and
swelling behavior in gas injection for the shale reservoir fluids under macro- to nano-scale porous geometries.
Advisors/Committee Members: Nasrabadi, Hadi (advisor), Lutkenhaus, Jodie L. (advisor), Killough, John (committee member), Gildin, Eduardo (committee member).
Subjects/Keywords: Phase behavior; Petroleum fluids
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
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APA (6th Edition):
Luo, S. (2018). Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/174434
Chicago Manual of Style (16th Edition):
Luo, Sheng. “Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/174434.
MLA Handbook (7th Edition):
Luo, Sheng. “Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media.” 2018. Web. 21 Apr 2021.
Vancouver:
Luo S. Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/174434.
Council of Science Editors:
Luo S. Experimental and Simulation Studies on Phase Behavior of Petroleum Fluids in Nanoporous Media. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/174434

Texas A&M University
10.
Lee, Jongbok.
Thermodynamic Synthesis of Ladder-Type Functional Organic Materials.
Degree: PhD, Chemistry, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/173939
► Conjugated ladder-type macromolecules with coplanar, sp2 atom-rich backbones represent a captivating class of materials on account of their well-defined rigid structures, intriguing syntheses, and promising…
(more)
▼ Conjugated ladder-type macromolecules with coplanar, sp2 atom-rich backbones represent a captivating class of materials on account of their well-defined rigid structures, intriguing syntheses, and promising potential in optoelectronic applications. The ladder-type backbones possess an intrinsically rigid conformation and limit possible torsional disorder. The unique architecture of conjugated ladder-type material leads to extended π-conjugation length, longer exciton diffusion length, and enhanced stability. In contrast, conventional conjugated polymers have intrinsic torsional disorder which partially break the conjugation pathways of the polymers and could be detrimental to the material properties.
Several preliminary literature examples have demonstrated the synthesis of ladder-type materials. However, it is still challenging to synthesize well-defined ladder polymers with a minimum level of structural defects because of the poor product solubility and limited synthetic methods. In order to overcome these obstacles, a highly efficient synthetic method and a rationally designed structural characteristic that enables solubility need to be accomplished simultaneously.
We envisioned that thermodynamically controlled ring-closing olefin metathesis (RCM) held the promise for a highly efficient and synthesis of conjugated ladder polymers with minimum levels of structural defects due to the strong thermodynamic driving force of aromatization and its reversible nature between starting material and side products. Moreover, the mild reaction conditions allow a wider scope of substrates and excellent
functional group tolerance. This efficient and versatile synthetic strategy successfully afforded various fused polycyclic heteroarenes, a series of extended ladder-type oligomers, and conjugated ladder polymers with minimum levels of structural defects in excellent yields. Furthermore, RCM demonstrated an excellent ring annulation efficiency with electron deficient acceptor units. Due to the good solubility of the ladder-type materials originating from orthogonally adopted α-branched solubilizing group, the properties of the desired materials were rigorously investigated in solution and the solid-state, such as photophysical properties, solid-state conformation and morphology, effective conjugation length, formation of charge transfer complexes, and crystallization dynamics. This research provides a well-established synthetic strategy to construct a fully conjugated ladder-type material and a fundamental understanding of ladder-type functional organic materials for potential future applications in electronic and optoelectronic devices.
Advisors/Committee Members: Fang, Lei (advisor), Darensbourg, Donald J (committee member), Wooley, Karen L (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: Ladder polymer; Ring-closing olefin metathesis; Thermodynamic synthesis; Ladderization; Fused-ring heteroarenes; Graphene nanoribbons
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Lee, J. (2018). Thermodynamic Synthesis of Ladder-Type Functional Organic Materials. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/173939
Chicago Manual of Style (16th Edition):
Lee, Jongbok. “Thermodynamic Synthesis of Ladder-Type Functional Organic Materials.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/173939.
MLA Handbook (7th Edition):
Lee, Jongbok. “Thermodynamic Synthesis of Ladder-Type Functional Organic Materials.” 2018. Web. 21 Apr 2021.
Vancouver:
Lee J. Thermodynamic Synthesis of Ladder-Type Functional Organic Materials. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/173939.
Council of Science Editors:
Lee J. Thermodynamic Synthesis of Ladder-Type Functional Organic Materials. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/173939
11.
Santos, Melissa Cruz.
Liquid Water Transport in Polymeric Films and Membranes.
Degree: PhD, Chemical Engineering, 2017, Texas A&M University
URL: http://hdl.handle.net/1969.1/161359
► Accurately measuring and understanding transport mechanisms of liquids in polymers is important for the development of materials used in applications such as packaging, water purification,…
(more)
▼ Accurately measuring and understanding transport mechanisms of liquids in polymers is important for the development of materials used in applications such as packaging, water purification, and corrosion protection.
In this work, an in situ pressure-contact Fourier transform infrared attenuated total reflectance (FTIR-ATR) spectroscopy apparatus was designed and developed for accurately measuring liquid water transport in free-standing polymer films. This new technique allows time-resolved infrared data of liquid transport in free-standing films to be collected accurately without solution casting the film directly onto the ATR element. Liquid transport in a rubbery polymer, glassy polymer, and a crosslinked polymer was measured and compared using this technique. The in situ pressure-contact FTIR-ATR spectroscopy apparatus showed similar results to those obtained using the conventional solution-cast FTIR-ATR apparatus for the rubbery polymer. Liquid water diffusion in the rubbery polymer exhibited non-Fickian behavior. Non-Fickian behavior was observed for the glassy polymer which was attributed to diffusion-relaxation and difference between the conventional solution-cast FTIR-ATR apparatus and the pressure-contact apparatus. Liquid water diffusion in the crosslinked polymer exhibited Fickian behavior and was attributed to the suppressed polymer strain response to the diffusant.
Diffusion in glassy polymers can be difficult to measure because of their nonequilibrium nature (i.e., Tg, of the polymer is much higher than the experimental temperature. In this work, the effect of glass transition temperature, Tg, on liquid water diffusion behavior in polymer-ionic liquid (IL) mixtures was investigated. Liquid water transport in glassy polymer-ionic liquid mixtures of varying IL content (0 to 50 w/w % IL) was studied to determine the effect of changing the glass transition temperature, Tg, on diffusion behavior. The results of this study showed that as IL content increased and Tg decreased, the liquid water diffusion behavior became more Fickian. This is because as Tg decreases, the free volume of the polymer increases, and the polymer approaches equilibrium.
Liquid water transport in polymers is also important for separations applications such as water purification. Recent research has focused on a promising hybrid technology, reactive electrochemical membranes (REMs) which act both as a membrane and a reactive electrochemical surface for the electrochemical degradation of pollutants However, they are limited by morphology, and therefore conductive REMs with tailored porosities are needed. In this study porous, flexible reactive electrochemical membranes (REMs) for water purification were synthesized by a novel simultaneous electrospinning/electrospraying (E/E) technique. The fabricated E/E REMs were durable, highly porous, and conductive membranes, performing comparably to carbon nanotube flow-through reactors, which are among the highest performing in literature. Further studies exploring the use of FTIR-ATR…
Advisors/Committee Members: Elabd, Yossef A (advisor), Lutkenhaus, Jodie L (committee member), Green, Micah J (committee member), Grunlan, Jaime C (committee member).
Subjects/Keywords: liquid diffusion; polymers; transport
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Santos, M. C. (2017). Liquid Water Transport in Polymeric Films and Membranes. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/161359
Chicago Manual of Style (16th Edition):
Santos, Melissa Cruz. “Liquid Water Transport in Polymeric Films and Membranes.” 2017. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/161359.
MLA Handbook (7th Edition):
Santos, Melissa Cruz. “Liquid Water Transport in Polymeric Films and Membranes.” 2017. Web. 21 Apr 2021.
Vancouver:
Santos MC. Liquid Water Transport in Polymeric Films and Membranes. [Internet] [Doctoral dissertation]. Texas A&M University; 2017. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/161359.
Council of Science Editors:
Santos MC. Liquid Water Transport in Polymeric Films and Membranes. [Doctoral Dissertation]. Texas A&M University; 2017. Available from: http://hdl.handle.net/1969.1/161359

Texas A&M University
12.
Hirai, Masato.
Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts.
Degree: PhD, Chemistry, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/157932
► It is known that SbF5 and SbCl5 are highly robust and show stronger acidic behavior than their boron counterparts, BF3 and BCl3, respectively. This effect…
(more)
▼ It is known that SbF5 and SbCl5 are highly robust and show stronger acidic behavior than their boron counterparts, BF3 and BCl3, respectively. This effect is caused by the polarizability and the electropositivity of these heavy elements as well as a lowering of the element-centered σ* orbitals. These larger elements are also able to accept more ligands in their coordination sphere, thus promoting Lewis base coordination. However, antimony pentahalides violently react with water to generate the corresponding hydrohalic acids, which limits the scope of applications in which they can be employed. By replacing the Sb-X (X = F or Cl) bonds with carbon and/or oxygen substituents, this corrosive nature of antimony pentahalide species could be suppressed and become significantly more stable. As a drawback, displacement of electron-withdrawing halide substituents may also result in a decrease of Lewis acidity. It is therefore significant to design organoantimony (V) species that bear sufficient ligand functionalities to balance both reactivity and stability. In this dissertation, we will present our recent developments of both neutral and cationic organoantimony (V) compounds as sensors for small anions specifically in aqueous media, reagents to activate molecules such as organic carbonyls, and potential ligands for heavy transition metals.
Advisors/Committee Members: Gabbai, Francois P (advisor), Darensbourg, Marcetta Y (committee member), Ozerov, Oleg V (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: Lewis acids; organoantimony; anion sensing; catalysis; main-group chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Hirai, M. (2016). Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/157932
Chicago Manual of Style (16th Edition):
Hirai, Masato. “Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts.” 2016. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/157932.
MLA Handbook (7th Edition):
Hirai, Masato. “Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts.” 2016. Web. 21 Apr 2021.
Vancouver:
Hirai M. Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts. [Internet] [Doctoral dissertation]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/157932.
Council of Science Editors:
Hirai M. Neutral and Cationic Organoantimony(V) Lewis Acids as Fluoride Receptors and Catalysts. [Doctoral Dissertation]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/157932

Texas A&M University
13.
An, Hyosung.
Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers.
Degree: PhD, Chemical Engineering, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/173514
► A conductive block copolymer binder P3HT-b-PEO was studied to form a flexible, tough, carbon-free hybrid battery cathode. Only 5 wt. % polymer was required to triple…
(more)
▼ A conductive block copolymer binder P3HT-b-PEO was studied to form a flexible, tough, carbon-free hybrid battery cathode. Only 5 wt. % polymer was required to triple the flexibility of V₂O₅, and electrodes comprised of 10 wt. % polymer had unusually high toughness (293 kJ/m3) and specific energy (530 Wh/kg), both higher than reduced graphene oxide paper electrodes. Addition of P3HT-b-PEO increased lithium-ion diffusion, eliminated cracking during cycling, and enhanced cyclability relative to V₂O₅ alone.
We compared the P3HT-b-PEO block copolymer binders with P3HT, PEO, and a P3HT/PEO homopolymer blend in carbon-free V₂O₅. The electrode with P3HT-b-PEO binder showed the highest capacity of 190 mAh/g at a 0.1 C-rate after over 200 cycles, a 2.5-fold improvement of that of pure V₂O₅, whereas P3HT, PEO, and the blend exhibited capacities of 139, 130, and 70 mAh/g. The unique architecture of P3HT-b-PEO, wherein P3HT and PEO blocks are covalently bonded, improved the uniform distribution of the conductive binders within the V₂O₅ structure, whereas the analogous P3HT/PEO blend suffers from phase separation.
We presented the strong effects of regioregularity and molecular weight of the P3HT block in P3HT-b-PEO on molecular conformation and electrochemical properties by comparing four different P3HT-b-PEOs of varying P3HT regioregularity (86-97%) and molecular weight (8-19 kDa) while the PEO block was kept the same (7 kDa) to isolate the influence of the P3HT block. Our data show that, as increasing regioregularity, the capacity of P3HT-b-PEO significantly increase and, as increasing molecular weight, the redox potential decreases. The underlying reasons for this finding are revealed by the characterizations of P3HT backbone conformation and chain packing.
Also, we studied highly stretchable conductive titanium carbide (MXene) multilayer coatings that can undergo extreme deformation while maintaining their electrical conductivity. The conductive and conformal MXene multilayer coatings that can undergo large-scale mechanical deformation while maintaining a conductivity as high as 2,000 S/
m. MXene multilayers were successfully prepared onto flexible polymer sheet, stretchable poly(dimethylsiloxane), nylon fiber, and glass. The coating showed a recoverable resistance response to bending (up to 2.5 mm bending radius) and stretching (up to 40% tensile strain).
Advisors/Committee Members: Lutkenhaus, Jodie L (advisor), Balbuena, Perla B (committee member), Elabd, Yossef A (committee member), Banerjee, Sarbajit (committee member).
Subjects/Keywords: Battery; Binders; Flexible conductors
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
An, H. (2018). Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/173514
Chicago Manual of Style (16th Edition):
An, Hyosung. “Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/173514.
MLA Handbook (7th Edition):
An, Hyosung. “Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers.” 2018. Web. 21 Apr 2021.
Vancouver:
An H. Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/173514.
Council of Science Editors:
An H. Conducting Diblock Copolymers as Multifunctional Binders for Lithium-Ion Batteries & Surface-Agnostic Highly Stretchable and Bendable Conductive MXene Multilayers. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/173514

Texas A&M University
14.
Press, Loren Paul.
High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes.
Degree: PhD, Chemistry, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/158080
► Over the last century, transition metal-catalyzed C-H functionalization has emerged as one of the most important topics in synthetic chemistry. One type of C-H functionalization,…
(more)
▼ Over the last century, transition metal-catalyzed C-H functionalization has emerged as one of the most important topics in synthetic chemistry. One type of C-H functionalization, known as C-H borylation, generates organoboron reagents directly from hydrocarbon substrates. The synthetic utility of organoboron compounds is well established and numerous systems have been developed for the catalytic C-H borylation of alkyl and aromatic substrates since the reaction was first conceived over 20 years ago, yet catalysts that support high TONs remain limited to a handful of examples. Here we present highly active POCOP iridium complexes for the catalytic C-H borylation of arenes. In favorable cases, TONs exceeding 10,000 have been observed. The synthesis and isolation of multiple complexes potentially relevant to catalysis permitted examination of several key elementary reactions. We found C-H activation at Ir(I) here is in contrast to the olefin-free catalysis with state-of-the-art Ir complexes supported by neutral bidentate ligands, where the C-H activating step is understood to involve trivalent Ir-boryl intermediates.
Next, we investigated the stoichiometric reactivity of a (POCOP)Ir(boryl)2 complex with various small molecules under thermolytic conditions. Transition metalboryl complexes are ubiquitous in the literature and have been identified as key intermediates in several critical chemical transformations including C-H borylation and hydroborylation chemistries. The (POCOP)Ir(boryl)2 complex was found to undergo several stoichiometric transformations including reduction of CO2 to CO, 1,2- diborylation of ethylene and the selective protonation of one boryl ligand.
The synthesis and characterization of novel POCS pincer complexes of nickel, palladium and iridium are described. The modular design of the POCS pincer ligand allowed the exploration of monomeric and bridging ligand designs akin to PNN and PCN complexes.
The selective B-H functionalization of the mono-anionic carborane [HCB11H11]^– with one or three triflyloxy (OTf) groups is described. The mono-triflyloxy substituted carborane can be halogenated to give pentabromo and decachloro derivatives with preservation of the B–OTf linkage. The use of [HCB11Cl10OTf]^– as a weakly coordinating anion is demonstrated.
Advisors/Committee Members: Ozerov, Oleg V. (advisor), Darensbourg, Donald J. (committee member), Hall, Michael B. (committee member), Lutkenhaus, Jodie L. (committee member).
Subjects/Keywords: C-H functionalization; C-H activation; borylation; POCOP; iridium; POCS; triflyloxy; carboranes; weakly coordinating anions
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Press, L. P. (2016). High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/158080
Chicago Manual of Style (16th Edition):
Press, Loren Paul. “High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes.” 2016. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/158080.
MLA Handbook (7th Edition):
Press, Loren Paul. “High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes.” 2016. Web. 21 Apr 2021.
Vancouver:
Press LP. High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes. [Internet] [Doctoral dissertation]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/158080.
Council of Science Editors:
Press LP. High-Turnover C-H Borylation of Arenes with (POCOP) Iridium Complexes, The Synthesis of Group 9/10 (POCS) Complexes and the Study of Triflyloxy-Substituted Carboranes. [Doctoral Dissertation]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/158080

Texas A&M University
15.
Jeon, Ju Won.
Charge Storage in Organic Electrodes for Energy & Electrochemical Applications.
Degree: PhD, Chemical Engineering, 2014, Texas A&M University
URL: http://hdl.handle.net/1969.1/153935
► Energy storage has been emerging as an important research topic because of the lack of fossil fuels and growing energy consumption. This thesis focuses on…
(more)
▼ Energy storage has been emerging as an important research topic because of the lack of fossil fuels and growing energy consumption. This thesis focuses on synthesis and characterization of electrode materials such as polyaniline, graphene, and nitrogen-doped porous carbon for use in energy storage applications.
Polyaniline (PANI), a conjugated polymer, has been widely investigated as an electrode material for energy storage. In order to enhance its oxidative stability, polyaniline:poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PANI:PAAMPSA) complex was synthesized using template polymerization. PANI:PAAMPSA possessed significantly increased oxidative stability up to 4.5 V (vs. Li/Li+) due to electrostatic and hydrogen bonding interactions between PANI and PAAMPSA. This polyacid-doped PANI showed a reversible capacity of 230 mAh/gPANI for over 800 cycles.
Three different polyaniline-based layer-by-layer (LbL) electrodes, PANI/PAAMPSA, PANI/PANI:PAAMPSA, and linear poly(ethylenimine)/PANI:PAAMPSA were fabricated and their charge storage natures were assessed in non-aqueous energy storage systems. PANI:PAAMPSA retained its oxidative stability within LbL electrodes. The PANI/PAAMPSA LbL electrode did not show enhanced oxidative stability as compared to PANI:PAAMPSA complexes, which indicates that the interactions between PANI and PAAMPSA are not as strong as in PANI:PAAMPSA complexes.
Porous PANI nanofiber/graphene hybrid electrodes were prepared by electrochemical reduction of PANI nanofiber/graphene oxide (PANI NF/GO) LbL assemblies at 1.5 V (vs. Li/Li+). The limited processibility of reduced graphene oxide was circumvented by using GO to build up PANI NF/GO LbL films followed by electrochemical reduction. PANI NF/electrochemically reduced graphene oxide (ERGO) LbL electrodes show high capacity and enhanced cycling stability. Its performance is strongly dependent on electrode thickness.
Nitrogen-doped porous carbon was synthesized by one-step carbonization of isorecticular metal-organic frameworks (IRMOF-3). Porous IRMOF-3 itself acts as a self-sacrificial template to provide porous structure. Furthermore, additional carbon and nitrogen sources were not required. The nitrogen content can be easily controlled by varying carbonization temperature. Nitrogen-doped porous carbon possessed significantly higher capacitance due to additional pseudocapacitance originating from nitrogen as compared to analogous nitrogen-free porous carbons.
Advisors/Committee Members: Lutkenhaus, Jodie L (advisor), Balbuena, Perla (committee member), Grunlan, Jamie (committee member), Wooley, Karen L (committee member).
Subjects/Keywords: Energy storage
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Jeon, J. W. (2014). Charge Storage in Organic Electrodes for Energy & Electrochemical Applications. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/153935
Chicago Manual of Style (16th Edition):
Jeon, Ju Won. “Charge Storage in Organic Electrodes for Energy & Electrochemical Applications.” 2014. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/153935.
MLA Handbook (7th Edition):
Jeon, Ju Won. “Charge Storage in Organic Electrodes for Energy & Electrochemical Applications.” 2014. Web. 21 Apr 2021.
Vancouver:
Jeon JW. Charge Storage in Organic Electrodes for Energy & Electrochemical Applications. [Internet] [Doctoral dissertation]. Texas A&M University; 2014. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/153935.
Council of Science Editors:
Jeon JW. Charge Storage in Organic Electrodes for Energy & Electrochemical Applications. [Doctoral Dissertation]. Texas A&M University; 2014. Available from: http://hdl.handle.net/1969.1/153935

Texas A&M University
16.
Boralugodage, Nilusha P.
End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis.
Degree: PhD, Chemistry, 2013, Texas A&M University
URL: http://hdl.handle.net/1969.1/150986
► Non-polar phase selectively soluble polyisobutylene (PIB) is a useful polymer as a polymer support for homogeneous catalysts. Substitution of PIB onto other useful ligands alters…
(more)
▼ Non-polar phase selectively soluble polyisobutylene (PIB) is a useful polymer as a polymer support for homogeneous catalysts. Substitution of PIB onto other useful ligands alters the solubility properties of original ligands. However, such chemical modification of PIB polymers is challenging due to its limited synthetic availability. This dissertation describes the end functionalization of this terminal alkene functionalized PIB into variety of other functional groups via variety of chemistries such as electrophilic aromatic substitutions, nucleophilic aromatic substitution reactions and alkylation reactions.
PIB-anilines and PIB-phenols can be prepared via electrophilic aromatic substitution reactions of anilines and phenols by PIB-alkene. Excellent oxidative and chemical resistance and nonpolar phase selective solubility of these modified PIB polymers allow these materials to be useful as soluble polymer supports for ligands and transition metal catalysts. This dissertation details immobilization of palladium and ruthenium catalysts on to these modified PIB ligands and their catalytic properties and catalyst recyclability. PIB-bound palladium catalyst was used as a recyclable homogeneous catalyst for cross coupling reactions in a thermomorphic liquid/liquid separation system- biphasic at a lower temperature and monophasic at a higher temperature. Application of a ‘solid solvent’-(Polywax) in place of a organic solvent is also described and improved metal sequestration of this liquid/solid catalyst/product separation compared to the thermomorphic liquid/liquid separation strategy is also investigated. A PIB-bound ruthenium visible light photo-redox catalyst was prepared and its catalytic activity and recyclability in free radical polymerization reactions of acrylates is also reported.
At the end this dissertation details the extension of PIB’s utility as a nonpolar phase anchor to functionalize polyolefins with dyes. This is illustrated by preparing PIB-bound metallophthalocyanine dyes in a series of reactions starting with 4-nitro phthalonitrile. The non-polar solvent solubility of these dyes allowed their use in dyeing commercial polyethylene and polypropylene.
Advisors/Committee Members: Bergbreiter, David E (advisor), Singleton, Daniel (committee member), Wooley, Karen L (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: polyisobutylene
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APA (6th Edition):
Boralugodage, N. P. (2013). End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/150986
Chicago Manual of Style (16th Edition):
Boralugodage, Nilusha P. “End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis.” 2013. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/150986.
MLA Handbook (7th Edition):
Boralugodage, Nilusha P. “End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis.” 2013. Web. 21 Apr 2021.
Vancouver:
Boralugodage NP. End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis. [Internet] [Doctoral dissertation]. Texas A&M University; 2013. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/150986.
Council of Science Editors:
Boralugodage NP. End Functinalization of Polyisobutylenes and their Applications in Dyeing Polyolefins and in Homogeneous Catalysis. [Doctoral Dissertation]. Texas A&M University; 2013. Available from: http://hdl.handle.net/1969.1/150986

Texas A&M University
17.
Cho, Chungyeon.
A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers.
Degree: PhD, Materials Science and Engineering, 2013, Texas A&M University
URL: http://hdl.handle.net/1969.1/151024
► This thesis research focuses on fundamental understanding regarding the morphological transitions of weak polyelectrolyte multilayers (PEMs) formed by the layer-by-layer (LbL) electrostatic assembly of oppositely…
(more)
▼ This thesis research focuses on fundamental understanding regarding the morphological transitions of weak polyelectrolyte multilayers (PEMs) formed by the layer-by-layer (LbL) electrostatic assembly of oppositely charged polymers.
he first part of this thesis focuses on patterning polyelectrolyte multilayers that are able to undergo transitions from continuous films to porous materials by using hydrogel stamps. The stamping process is able to locally etch and pattern the porous transition in the LbL films by using reactive wet stamping (r-WETS). It was found that r-WETS of PEMs can also enable the modification of chemical functionality.
The second part is an investigation about morphological changes of weak polyelectrolyte multilayers assembled with PAH and PAA using r-WETS in which hydrogel stamp material was soaked into various salt solutions and then applied to the LbL films. Also, in this study we presented a novel strategy to create a continuous gradient structure in thickness or porosity along the lateral direction of the thin films using concentration gradient salt stamping.
The third part is an investigation regarding the mechanism of the transition from a continuous morphology to a porous morphology within weak polyelectrolyte multilayers. These morphological changes were able to be created by both acidic and basic post-assembly treatments, showing various morphological transitions from the introduction of porosity to the collapse of these porous structures and the eventual dissolution of the films.
A similar observation of morphological transitions in weak polyelectrolyte multilayers was obtained by applying an electric field to the films in the fourth part of this thesis. Exposure to an electric field resulted in the creation of a porous structure, which can be ascribed to local changes in pH and subsequent structural rearrangements of the weak polyelectrolyte constituents.
The final part of this thesis is to make PEMs into nanostructured matrices for inorganic synthesis. Multilayers possessing ion-exchangeable carboxylic acid groups were used for binding metal catalysts such as platinum (Pt) nanoparticles (NPs) within the film. Therefore, polyelectrolyte multilayers were able to stabilize catalytic Pt NPs in order to increase the useful time of catalyst materials suitable for use in proton exchange membrane fuel cells.
Advisors/Committee Members: Nicole, Zacharia S (advisor), Lutkenhaus, Jodie L (committee member), Akbulut, Mustafa (committee member), Vaddiraju, Sreeram (committee member).
Subjects/Keywords: Polyelectrolytes; Layer-by-Layer method; Post-Assembly Treatment; Porous Transitions; Reactive Wet Stamping
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
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APA (6th Edition):
Cho, C. (2013). A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/151024
Chicago Manual of Style (16th Edition):
Cho, Chungyeon. “A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers.” 2013. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/151024.
MLA Handbook (7th Edition):
Cho, Chungyeon. “A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers.” 2013. Web. 21 Apr 2021.
Vancouver:
Cho C. A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers. [Internet] [Doctoral dissertation]. Texas A&M University; 2013. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/151024.
Council of Science Editors:
Cho C. A Study of Porous Transitions of Layer-By-Layer Thin Films and Patterning Multilayers. [Doctoral Dissertation]. Texas A&M University; 2013. Available from: http://hdl.handle.net/1969.1/151024

Texas A&M University
18.
Pavia Sanders, Adriana.
Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems.
Degree: PhD, Chemistry, 2015, Texas A&M University
URL: http://hdl.handle.net/1969.1/156379
► Environmental remediation of pollutants from water systems is an expanding billion dollar industry. Recently, engineered nanoparticles (ENPs) have been of particular interest to this field…
(more)
▼ Environmental remediation of pollutants from water systems is an expanding billion dollar industry. Recently, engineered nanoparticles (ENPs) have been of particular interest to this field as they hold promise in improving existing remediation technologies. Hybrid well-defined magnetic shell crosslinked knedel-like (MSCK) nanoparticles comprised of iron oxide nanoparticles encapsulated in amphiphilic block copolymer micellar assemblies and selectively crosslinked throughout the hydrophilic shell domain of the assembly have been investigated for their pollutant uptake capabilities. The main focus of this dissertation is to design, develop, and investigate tailored MSCK nanoparticle systems for specific environmental pollutants and applications.
Alterations of the polymeric components of the nanoparticle systems allow for the development of fine-tuned materials by providing control over the composition, shape, and size of the nanoparticles produced. The polymeric components utilized for the co-assemblies of the MSCK systems presented here were produced through two types of controlled living radical polymerizations, atom transfer radical polymerization (ATRP) and reversible addition-fragmentation chain-transfer (RAFT) polymerization. The non-covalent incorporation of iron oxide nanoparticles into the cores of the systems was performed in order to afford magnetically active materials that can be controlled and/or recovered after deployment through the use of an external magnetic field. In order to achieve a high magnetic response, the co-assemblies of these systems were achieved with equal mass feed ratios of the polymers and iron oxide nanoparticles during the micellization process. MSCKs designed for their utilization following the bulk recovery stage at oil spill sites to recover oil at low concentrations, or sheen, were composed of poly(acrylic acid)20-b-polystyrene280 (PAA20-b-PS280) and demonstrated superb sheen recovery of ten-fold by weight. Fluorinated MSCK (MSCK-F9) nanoparticles were also investigated for the remediation of perfluorooctanoic acid (PFAO) from water. A library of four fluorinated systems was developed in order to probe the effect size/fluorine content and shell charge would have on the recovery efficiency of these materials. A fluorinated monomer was incorporated into the polymer during polymerization in order to increase the solvation of PFOA within the core during loading. The results of this dissertation suggest that MSCKs are a viable option and ENPs for environmental remediation.
Advisors/Committee Members: Wooley, Karen L (committee member), Singleton, Daniel A (committee member), Fang, Lei (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: Hybrid; Polymer; Nanoremediation; MSCK; Crude oil; PFOA
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
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APA (6th Edition):
Pavia Sanders, A. (2015). Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/156379
Chicago Manual of Style (16th Edition):
Pavia Sanders, Adriana. “Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems.” 2015. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/156379.
MLA Handbook (7th Edition):
Pavia Sanders, Adriana. “Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems.” 2015. Web. 21 Apr 2021.
Vancouver:
Pavia Sanders A. Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems. [Internet] [Doctoral dissertation]. Texas A&M University; 2015. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/156379.
Council of Science Editors:
Pavia Sanders A. Hybrid Magnetic Polymerica Nanoparticles for the Environmental Remediation of Crude Oil and Perfluorooctanoic Acid from Aqueous Systems. [Doctoral Dissertation]. Texas A&M University; 2015. Available from: http://hdl.handle.net/1969.1/156379

Texas A&M University
19.
Kyran, Samuel John.
Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes.
Degree: PhD, Chemistry, 2015, Texas A&M University
URL: http://hdl.handle.net/1969.1/156382
► Small molecules carbon dioxide and carbon monoxide produced via the oxidation and partial oxidation of carbonaceous matter, respectively, have distinct chemical functions and reactivity. A…
(more)
▼ Small molecules carbon dioxide and carbon monoxide produced via the oxidation and partial oxidation of carbonaceous matter, respectively, have distinct chemical functions and reactivity. A fairly stable species and a greenhouse gas, carbon dioxide has risen to an unprecedented level of 400 ppm in the atmosphere by the increased consumption of fossil fuels. To address this undesired accumulation of carbon dioxide, various solutions are being introduced and the utilization of carbon dioxide as a C1 feedstock in chemical synthesis can contribute towards this goal. The levels of carbon monoxide are unaffected as it is relatively short-lived in the atmosphere and is considered a temporary pollutant. High concentrations are toxic to humans due to its ability to displace oxygen from red blood cells. Nanomolar concentrations of carbon monoxide, however, are endogenously-produced and are beneficial to physiology due to its unexpected role as a regulatory molecule. Herein, results on various chemical transformations of carbon dioxide and studies on reactions involving carbon monoxide are presented.
A promising endeavor is the synthesis of polycarbonates from carbon dioxide and epoxides. The use of a naphthalene derived epoxide to produce poly(1,4-dihydronaphthalene carbonate) exhibiting high thermal transitions comparable to bisphenol-A polycarbonate is illustrated. Being a large monomer, employing traditional tert-butyl substituted (salen)Cr(III) catalysts show poor polymer selectivity, whereas the use of a planar tetraazaannulene bound Cr(III) catalyst is successful in chain propagation and subsequently displays higher activity. Fundamental studies on direct carboxylation of hydrocarbons were also investigated. Carbon dioxide insertions into Ru-H and Ru-Me bonds proceed favorably at electron rich metal centers and the formation of an acetate is thermodynamically more stable when compared with formate formation. Bond dissociation energies of acrylates from ruthenium and iron complexes, prepared synthetically as model compounds of an ethylene and carbon dioxide coupled product, were measured through kinetic experiments. Ruthenium complexes show lower BDEs.
Rhenium and manganese carbonyls bound by a hemi-labile pyrrolyl carboxyaldehyde and a bulky diazabutadiene ligand, respectively, are evaluated as carbon monoxide releasing molecules. Additionally, a detailed mechanistic investigation on an unusual carbon monoxide reaction with a synthetic analogue of a biomimetic iron dinitrosyl complex is described.
Advisors/Committee Members: Darensbourg, Donald J (advisor), Gabbaï, François P (committee member), Ozerov, Oleg V (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: carbon dioxide; epoxides; polycarbonates; CO2 insertion chemistry; acrylic acid; carbon monoxide releasing molecules; dinitrosyl iron complexes
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
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APA (6th Edition):
Kyran, S. J. (2015). Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/156382
Chicago Manual of Style (16th Edition):
Kyran, Samuel John. “Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes.” 2015. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/156382.
MLA Handbook (7th Edition):
Kyran, Samuel John. “Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes.” 2015. Web. 21 Apr 2021.
Vancouver:
Kyran SJ. Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes. [Internet] [Doctoral dissertation]. Texas A&M University; 2015. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/156382.
Council of Science Editors:
Kyran SJ. Activation of Carbon Oxides: Chemical Reactions and Transformations Facilitated by Groups 6, 7, & 8 Metal Complexes. [Doctoral Dissertation]. Texas A&M University; 2015. Available from: http://hdl.handle.net/1969.1/156382

Texas A&M University
20.
Yang, Haifeng.
Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis.
Degree: PhD, Chemistry, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/158094
► Ligand design has been an often pursued strategy to advance the development of transition metal complexes for catalysis and activation of small molecules. In the…
(more)
▼ Ligand design has been an often pursued strategy to advance the development of transition metal complexes for catalysis and activation of small molecules. In the past decade, polydentate Z-type ligands have been recognized as versatile tools to expand on the reactivity of transition metals. The interest generated by polydentate Z-type ligands mainly arises from the ability of the Lewis acidic Z site to behave as σ-acceptor, which can modulate the electronic properties of the metal and impart reactivity to the metal via flexible metal→Z ligand interaction. Group 13 compounds, notable for their Lewis acidity, have been dominating the field of Z-type ligand chemistry, leading to a plethora of discoveries in small molecules activation and organic transformation catalysis.
In recent years, heavy main group antimony and tellurium compounds made their unique entry into the Z-type ligand family owing to their Lewis acidity and redox activity. In particular, it was demonstrated that weak donating stibine and telluroether ligands can be switched into σ-accepting Z-type ligands by post-synthetic conversion to their hyper-valent state. Although these phenomena are of fundamental importance, attempts to use these metal complexes for metal catalyzed processes or chemical transformations have not been explored. To fill this knowledge gap, it became the objective of this dissertation to investigate new versions of antimony or tellurium ligand systems and probe their use for the design of late transition metal-based catalysts
With this in mind, I chose to investigate halogen functionalized antimony ligands, with augmented Lewis acidity due to the electronegativity of the halogen atoms. The strong Lewis acidity of the halostibine antimony center, coupled with its capacity to undergo oxidation reactions or anion exchanges, led to the isolation of trihalostiborane-gold complexes and trihalostiborane-platinum complexes, featuring magnified metal→Sb(V) interactions. These complexes have been exploited in the development of ligand-centered redox-controlled catalysis, highlighting their utility in the area of smart catalyst design. Another noteworthy result of this research includes the discovery of redox active antimony-platinum molecular platform, in which the halogenated antimony ligand is able to modulate the electron density of the coordinated platinum, thereby facilitating the two-electron redox reactions. Such redox reactions have been utilized to realize the high-quantum-yield photoreductive elimination of chlorine, which is of relevance to photocatalytic production of H2 from HX. In parallel to the antimony chemistry, tellurium ligand chemistry has also been investigated. Our results in this area show for the first time the redox non-innocent behavior of telluroether ligand in the coordination sphere of gold.
Advisors/Committee Members: Gabbaï, François P (advisor), Hall, Michael B (committee member), Ozerov, Oleg V (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: Z-type ligands; Redox non-innocent; Coordination non-innocent; Antimony; Tellurium; Platinum; Gold; Photoreductive elimination; Catalysis
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APA ·
Chicago ·
MLA ·
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CSE |
Export
to Zotero / EndNote / Reference
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APA (6th Edition):
Yang, H. (2016). Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/158094
Chicago Manual of Style (16th Edition):
Yang, Haifeng. “Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis.” 2016. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/158094.
MLA Handbook (7th Edition):
Yang, Haifeng. “Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis.” 2016. Web. 21 Apr 2021.
Vancouver:
Yang H. Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis. [Internet] [Doctoral dissertation]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/158094.
Council of Science Editors:
Yang H. Antimony and Tellurium Non-Innocent Z-Ligands for Transition Metals and Their Application in Photoredox Chemistry and Electrophilic Catalysis. [Doctoral Dissertation]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/158094

Texas A&M University
21.
Li, Richen.
Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications.
Degree: PhD, Chemistry, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/174598
► Degradable polymers have gained increasing interest in the molecular probe and nanomedicine research, which avoid safety concerns of non-degradable materials after long-term accumulation in the…
(more)
▼ Degradable polymers have gained increasing interest in the molecular probe and nanomedicine research, which avoid safety concerns of non-degradable materials after long-term accumulation in the human body. This dissertation focuses on the rational design and synthesis of biocompatible polymers, based on polyphosphoesters (PPEs) and poly(glucose carbonate)s (PGCs), which are capable of serving as non-immunotoxic antifouling coatings for molecular nanoprobes to accurately image tumors, or formulating well-defined functional nanocarriers for therapeutics to effectively treat osteosarcoma lung metastasis or bacterial infections.
In the first study, zwitterionic PPEs (zPPEs) were developed as coating materials for gold nanoparticles (AuNPs), which showed minimal immunotoxicity and advanced antifouling property. The PPE was synthesized by a rapid organocatalyzed ring-opening polymerization (ROP), followed by post-polymerization modification via the thiol-yne click reaction to afford the zPPEs. Degradability of the zPPEs was investigated in nanopure water (pH 5-6), which proceeded to ca. 75% after 2 d, and ca. 90% by 7 d, consistent with the degradation profiles of the zPPE-coated AuNPs. Compared to their counterparts coated with poly(ethylene glycol) (PEG), the zPPE-coated AuNPs showed similar sizes and low immunotoxicity. Moreover, significantly reduced cytokine adsorption was observed for the zPPE-coated nanoparticles. The degradability, biocompatibility and advanced antifouling property demonstrate the zPPE to be a potential PEG alternative coating material for molecular nanoprobes.
To circumvent potential drawbacks of our previous PPE system, namely the production of ethylene glycol and phosphoric acid upon hydrolytic degradation, sugar-derived PGC-based polymers were developed in the second study, which was utilized to formulate functional
nanocarriers for anticancer drugs to treat osteosarcoma (OS) lung metastases. Two PGC-based block polymers and one dimeric paclitaxel pro-drug (diPTX) were designed to be co-assembled into nanoparticles with tunable sizes and surface charges as a redox-responsive nanomedicine. The formulation showed sustained release of the PTX free drug in the presence of glutathione, a reducing agent existing at high levels in tumor tissues, thereby resulting in significant selectivity in killing cancer cells over healthy cells. Both in vitro and in vivo anticancer studies confirmed the capability of the formulation to penetrate tumor tissues and inhibit tumor cell growth, indicating its promise for the treatment of OS lung metastases.
In the third study, a novel PPE-based triblock polymer was designed and synthesized, which avoided the hydrolytic degradation product ethylene glycol, and allowed for facile construction of silver-loaded Janus nanoparticles as a potential antimicrobial. The polymer was synthesized by a one-pot sequential organocatalyzed ROP of a cyclic phosphotriester and
L-lactide with PEG as the macroinitiator, followed by post-polymerization modification via the thiol-ene…
Advisors/Committee Members: Wooley, Karen L. (advisor), Darensbourg, Marcetta Y. (committee member), Lutkenhaus, Jodie L. (committee member), Zhou, Hongcai (committee member).
Subjects/Keywords: Degradable polymer; imaging; drug delivery
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APA ·
Chicago ·
MLA ·
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CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Li, R. (2018). Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/174598
Chicago Manual of Style (16th Edition):
Li, Richen. “Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/174598.
MLA Handbook (7th Edition):
Li, Richen. “Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications.” 2018. Web. 21 Apr 2021.
Vancouver:
Li R. Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/174598.
Council of Science Editors:
Li R. Development of Degradable Polymeric Nanoscopic Platforms for Imaging and Drug Delivery Applications. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/174598

Texas A&M University
22.
Yang, Mengxi.
Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts.
Degree: PhD, Chemistry, 2018, Texas A&M University
URL: http://hdl.handle.net/1969.1/192057
► Organoantimony(V) compounds are potent Lewis acids which have been used for the complexation of anions or for the catalysis of organic reactions. Inspired by the…
(more)
▼ Organoantimony(V) compounds are potent Lewis acids which have been used for the complexation of anions or for the catalysis of organic reactions. Inspired by the broad range of applications developed for the stable Group 13 Lewis acid B(Cv6Fv5)v3, as well as the fact that SbFv5 is more acidic than BFv3, we set out to investigate organoantimony compounds in the context of Lewis acid catalysis. To this end, we synthesized electrophilic Sb(III) and Sb(V) complexes featuring electron-withdrawing halogenated ligands, cationic charges, and/or ancillary donor ligands, and tested these compounds in a number of organic transformations. Computational studies of their electronic structures provided us with insights into their unusual properties.
We compared a series of triarylstibines with their tetrachlorocatecholate stiborane analogs, and demonstrated that the Lewis acidity of organoantimony(III) species can be readily enhanced by oxidation to the +V state, a phenomenon that is rationalized by the lowering of the antimony-based accepting Ó* orbital and a “deepening” of the associated Ó-hole upon oxidation. We also reported the synthesis of triarylfluoro- and triarylchloro- stibonium cations, among which the trimesitylchlorostibonium hexachloroantimonate is free from direct cation-anion interactions due to the steric shielding provided by the mesityl substituents. However, this cation is not as reactive as its phenyl derivative in the catalytic polymerization of THF and the Friedel-Craft dimerization of 1,1-diphenlyethylene. Additionally, we evaluated a series of tetraarylstibonium cations as catalysts for the cycloaddition of isocyanates to oxiranes. While all stibonium cations
favor the 3,4-oxazolidinone products, the bulkier cations are found to be the most selective. Furthermore, we compared a series of ortho-phenylene based pnictogen cations and dications with their monofunctional derivatives as catalysts for the transfer hydrogenation of quinone derivatives with Hantzsch ester, and found that their catalytic reactivity follows the Lewis acidity trend in the order Sb dication > Sb monocation > P monocation. Lastly, this dissertation also investigates the electronic structures of selected organoantimony(V) compounds with the view to understand how coordination events at the antimony center affect the photophysical properties of these compounds.
Advisors/Committee Members: Gabbai, Francois P (advisor), Hall, Michael B (committee member), Nippe, Michael (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: antimony; Lewis acids; catalysis; molecular recognition; main-group
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Yang, M. (2018). Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/192057
Chicago Manual of Style (16th Edition):
Yang, Mengxi. “Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts.” 2018. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/192057.
MLA Handbook (7th Edition):
Yang, Mengxi. “Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts.” 2018. Web. 21 Apr 2021.
Vancouver:
Yang M. Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts. [Internet] [Doctoral dissertation]. Texas A&M University; 2018. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/192057.
Council of Science Editors:
Yang M. Neutral and Cationic Organoantimony Compounds as Lewis Acid Catalysts. [Doctoral Dissertation]. Texas A&M University; 2018. Available from: http://hdl.handle.net/1969.1/192057
23.
Hwang, Monica.
Ultra-Low Platinum and Platinum-Free Fuel Cells.
Degree: PhD, Chemical Engineering, 2019, Texas A&M University
URL: http://hdl.handle.net/1969.1/184918
► Fuel cells are attractive alternative energy sources due to their low-to-moderate operating temperature, zero greenhouse emission, and wide range of applications including automobiles and stationary…
(more)
▼ Fuel cells are attractive alternative energy sources due to their low-to-moderate operating temperature, zero greenhouse emission, and wide range of applications including automobiles and stationary power sources. However, they have key commercialization disadvantages. Proton exchange membrane fuel cells (PEMFCs) produce high power density but require expensive rare noble metal catalysts (e.g., platinum), which impedes PEMFC commercialization. Alkaline fuel cells (AFCs) are unstable and dangerous due to the use of caustic liquid electrolyte; therefore, solid-state membranes are necessary to promote safe, commercial AFCs. In this study, alternative electrode fabrication techniques and alternative hydrocarbon-based polymers as membranes and ionomers were explored to reduce the overall fuel cell cost for PEMFCs and AFCs.
Ultra-low platinum electrodes fabricated via electrospinning/electrospraying (E/E) produced higher PEMFC power density than conventional electrodes and provided insight in the ionomer impact on catalyst particle aggregates. To commercially fabricate E/E electrodes, a needleless electrospinning apparatus was developed in our laboratory. Needleless electrospinning produced proton-conducting nanofibers with higher mechanical and ion transport properties at a higher production rate than needle electrospinning due to multiple higher local polymer concentration sites at the electrospinning surface. Needleless electrospun nanofibers with catalyst particles were employed as ultra-low platinum loading fuel cell electrodes and demonstrated similar power densities as E/E electrodes. These results demonstrate the possibility of producing ultra-low platinum loading E/E electrodes at high production rates.
Commercially available pentablock terpolymers (PTPs) were used as membranes and ionomers in PEMFCs and AFCs. Sulfonated PTPs as membranes and ionomers demonstrated higher conductivity properties and reasonable power densities compared to the commercial fluorinated polymer (Nafion). Brominated and quaternized PTPs with methylpyrrolidinium cations were also developed as solid-state anion exchange membranes and demonstrated promising power densities and durability in AFC applications. Low-platinum E/E electrodes of electrospun PTP nanofibers and electrosprayed catalyst particles demonstrated better platinum utilization than conventional electrodes. The combination of commercial fabrication of ultra-low platinum E/E electrodes and commercially available low-cost ion exchange membranes and ionomers offer an affordable, sustainable, clean energy solution.
Advisors/Committee Members: Elabd, Yossef A (advisor), Lutkenhaus, Jodie L (committee member), Green, Micah J (committee member), Grunlan, Jaime C (committee member).
Subjects/Keywords: low-cost; polymer; stable
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APA (6th Edition):
Hwang, M. (2019). Ultra-Low Platinum and Platinum-Free Fuel Cells. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/184918
Chicago Manual of Style (16th Edition):
Hwang, Monica. “Ultra-Low Platinum and Platinum-Free Fuel Cells.” 2019. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/184918.
MLA Handbook (7th Edition):
Hwang, Monica. “Ultra-Low Platinum and Platinum-Free Fuel Cells.” 2019. Web. 21 Apr 2021.
Vancouver:
Hwang M. Ultra-Low Platinum and Platinum-Free Fuel Cells. [Internet] [Doctoral dissertation]. Texas A&M University; 2019. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/184918.
Council of Science Editors:
Hwang M. Ultra-Low Platinum and Platinum-Free Fuel Cells. [Doctoral Dissertation]. Texas A&M University; 2019. Available from: http://hdl.handle.net/1969.1/184918
24.
Meek, Kelly Marie.
Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes.
Degree: PhD, Chemical Engineering, 2016, Texas A&M University
URL: http://hdl.handle.net/1969.1/157003
► Non-platinum (low-cost), long-lasting, solid-state alkaline fuel cells (AFCs) require anion exchange membranes (AEMs) that have high alkaline chemical stability, high hydroxide ion conductivity, and adequate…
(more)
▼ Non-platinum (low-cost), long-lasting, solid-state alkaline fuel cells (AFCs) require anion exchange membranes (AEMs) that have high alkaline chemical stability, high hydroxide ion conductivity, and adequate mechanical properties. In this study, polymerized ionic liquid (PIL) block copolymers were explored as a viable candidate for AFCs. PIL block copolymers are an emerging class of polymers that synergistically combine the benefits of both ionic liquids and block copolymers into one, where the former possesses a unique set of physiochemical properties and the latter self assembles into a range of nanostructures. More importantly, the potential to synthesize a vast array of new block copolymers is almost limitless with numerous IL cations and anions available.
PIL diblock copolymers were first synthesized at various compositions from an imidazolium-based ionic liquid monomer and a non-ionic monomer via reverse addition fragmentation chain transfer polymerization. Hydroxide ion conductivities were higher in the PIL diblock copolymers compared to the analogous PIL homopolymer due to the nanostructured morphology in the PIL diblock copolymers. This demonstrates the high hydroxide ion conductivity of PIL block copolymers.
Numerous PILs were then synthesized with various covalently attached cations (butylimidazolium, butylmethylimidazolium, trimethylammonium, butylpyrrolidinium, trimethylphosphonium) and various backbone/cation pairings (backbones: ethyl methacrylate, undecyl methacrylate, undecyl acrylate, styrene; covalently attached cations: butylimidazolium, trimethylammonium, butylpyrrolidinium) and their alkaline chemical stability was carefully quantified with
1H NMR spectroscopy. The styrene/butylpyrrolidinium pairing proved to be highly chemically stable, with no degradation in 20 meq of KOH at 60 °C for 168 h.
Considering the high hydroxide conductivities of PIL block copolymers, and the high alkaline chemical stability of the styrene/pyrrolidinium-based PIL, conductivity and chemical stability of a PIL block copolymer (ABCBA pentablock terpolymer) with a styrene/pyrrolidinium-based PIL block was investigated. A high hydroxide conductivity of 43.4 mS cm
-1 at 60 °C in liquid water was achieved and no degradation or loss of conductivity was observed in the membrane after 168 h in 1
M KOH at 60 °C. PIL block copolymers utilizing a styrene/pyrrolidinium backbone/cation pairing in the PIL block represent a promising chemistry for producing highly conductive, chemically stable, robust AEMs for implementation in future solid-state AFCs.
Advisors/Committee Members: Elabd, Yossef A (advisor), Lutkenhaus, Jodie L (committee member), Cheng, Zheng Dong (committee member), Fang, Lei (committee member).
Subjects/Keywords: block copolymers; ion transport; ion conductivity; anion exchange membranes; alkaline chemical stability
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Meek, K. M. (2016). Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/157003
Chicago Manual of Style (16th Edition):
Meek, Kelly Marie. “Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes.” 2016. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/157003.
MLA Handbook (7th Edition):
Meek, Kelly Marie. “Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes.” 2016. Web. 21 Apr 2021.
Vancouver:
Meek KM. Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes. [Internet] [Doctoral dissertation]. Texas A&M University; 2016. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/157003.
Council of Science Editors:
Meek KM. Alkaline Chemical Stability and Ion Transport in Polymerized Ionic Liquid Anion Exchange Membranes. [Doctoral Dissertation]. Texas A&M University; 2016. Available from: http://hdl.handle.net/1969.1/157003
25.
Shi, Nan.
Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis.
Degree: PhD, Chemical Engineering, 2014, Texas A&M University
URL: http://hdl.handle.net/1969.1/153828
► Many efforts to develop advanced medical diagnostic capabilities rely on the ability to perform size-based separations of DNA and proteins. Miniaturized formats have potential to…
(more)
▼ Many efforts to develop advanced medical diagnostic capabilities rely on the ability to perform size-based separations of DNA and proteins. Miniaturized formats have potential to provide rapid integrated solutions, but rational development requires an improved understanding of the physics underlying separation. This dissertation majorly focuses on the DNA transport in microchip gel electrophoresis systems. We have developed a transport model that allows us to determine the interplay between the hydrogel pore size distribution, the applied electric field strength, and DNA size in determining separation performance. This fundamental understanding makes it possible to access a unique DNA transport mode, entropic trapping, that becomes dominant when the hydrogel pore size is close that of DNA coil. Further investigation of the entropic trapping phenomena, both experimentally and computationally, shows how the inherently disordered dynamics governing macromolecular transport under nanoconfined surroundings can paradoxically be precisely controlled. This capability lays a foundation for a sensitive probe of nanoscale molecular conformation, revealing previously unseen details about DNA-protein binding interactions at size scales far below the limits of conventional techniques. A key breakthrough is that our method is the first practical application of stochastic resonance in entropic trapping transport of macromolecules (previously studied, but only theoretically), yielding a new tool to “image” nanoscale details of biomolecular conformation.
Advisors/Committee Members: Ugaz, Victor M (advisor), Cheng, Zhengdong (committee member), Cagin, Tahir (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: DNA; Microchip; Gel electrophoresis
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Shi, N. (2014). Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/153828
Chicago Manual of Style (16th Edition):
Shi, Nan. “Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis.” 2014. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/153828.
MLA Handbook (7th Edition):
Shi, Nan. “Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis.” 2014. Web. 21 Apr 2021.
Vancouver:
Shi N. Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis. [Internet] [Doctoral dissertation]. Texas A&M University; 2014. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/153828.
Council of Science Editors:
Shi N. Investigation of the Effect of Hydrogel Pore Morphology on DNA Migration Mechanisms in Microchip Gel Electrophoresis. [Doctoral Dissertation]. Texas A&M University; 2014. Available from: http://hdl.handle.net/1969.1/153828
26.
Christianson, Anna Marie.
Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses.
Degree: PhD, Chemistry, 2017, Texas A&M University
URL: http://hdl.handle.net/1969.1/161393
► The design of molecular chemical sensors has generally relied on the use of colored and/or luminescent organic dyes or transition metal complexes; however, recent advances…
(more)
▼ The design of molecular chemical sensors has generally relied on the use of colored and/or luminescent organic dyes or transition metal complexes; however, recent advances have been made in the use of heavy main group elements such as phosphorus, selenium, antimony, and tellurium as functional elements in sensors. We have become interested in the use of heavy Group 15 elements for sensing, especially Lewis acidic organoantimony(V) derivatives, which may be used for the selective sensing of fluoride anions in water. Building upon our previous work, we have now developed a series of heavy Group 15-incorporating compounds featuring improved photophysical properties including visible-wavelength absorption and high quantum yield emission, sensitivity to a wider range of analytes for sensing, and a diverse manifold of sensing response mechanisms based on chemistry at the main group element. We have focused on uncovering these mechanisms through structural analysis and spectroscopic characterization supported by DFT computational methods, in order to gain understanding of the link between analyte recognition at the Group 15 element and the observed photophysical change.
To this end, we have synthesized and characterized antimony(III)- and antimony(V)-substituted derivatives of highly fluorescent BODIPY and fluorescein dyes, as well as intensely colored ruthenium polypyridyl complexes. The Lewis acidic Sb(V)-decorated BODIPY displays a “turn-on” fluorescent response to both fluoride and cyanide anions, while the Sb(III)-decorated fluorescein derivative functions as a “turn- off” sensor for peroxide. The Sb(V)-substituted ruthenium polypyridyl complex also responds to fluoride and cyanide anions, with a response that is observable both colorimetrically and electrochemically. A phosphorus-decorated fluorescein derivative has also been developed as a “turn-on” fluorescent sensor for gold(III) ions in aqueous solution, which is functional at nanomolar concentrations of gold. Finally, a series of Sb(III)- and Sb(V)-incorporating heterocycles have been developed that feature direct interaction of antimony-based σ* orbitals with the organic π system. In these compounds, the incorporation of antimony within the π-conjugated structure provides direct control over the photophysical properties, which holds promise for the design of anion sensors as well as color-tunable materials.
Advisors/Committee Members: Gabbai, Francois P (advisor), Darensbourg, Donald J (committee member), Ozerov, Oleg V (committee member), Lutkenhaus, Jodie L (committee member).
Subjects/Keywords: antimony; phosphorus; main group; chemical sensing; Lewis acids; fluorescence
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Christianson, A. M. (2017). Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/161393
Chicago Manual of Style (16th Edition):
Christianson, Anna Marie. “Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses.” 2017. Doctoral Dissertation, Texas A&M University. Accessed April 21, 2021.
http://hdl.handle.net/1969.1/161393.
MLA Handbook (7th Edition):
Christianson, Anna Marie. “Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses.” 2017. Web. 21 Apr 2021.
Vancouver:
Christianson AM. Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses. [Internet] [Doctoral dissertation]. Texas A&M University; 2017. [cited 2021 Apr 21].
Available from: http://hdl.handle.net/1969.1/161393.
Council of Science Editors:
Christianson AM. Organoantimony and Organophosphorus Compounds for Chemical Sensing: Toward Designed Fluorimetric and Colorimetric Responses. [Doctoral Dissertation]. Texas A&M University; 2017. Available from: http://hdl.handle.net/1969.1/161393
.