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Articles 1 - 30 of 54
Full-Text Articles in Physical Sciences and Mathematics
Reactive Chemistries For Protein Labeling, Degradation, And Stimuli Responsive Delivery, Myrat Kurbanov
Reactive Chemistries For Protein Labeling, Degradation, And Stimuli Responsive Delivery, Myrat Kurbanov
Doctoral Dissertations
Reactive chemistries for protein chemical modification play an instrumental role in chemical biology, proteomics, and therapeutics. Depending on the application, the selectivity of these modifications can range from precise modification of an amino acid sequence by genetic manipulation of protein expression machinery to a stochastic modification of lysine residues on the protein surface. Ligand-Directed (LD) chemistry is one of the few methods for targeted modification of endogenous proteins without genetic engineering. However, current LD strategies are limited by stringent amino acid selectivity. To bridge this gap, this thesis focuses on the development of highly reactive LD Triggerable Michael Acceptors (LD-TMAcs) …
Behavioral Modulation Of Supramolecular Assemblies Via Covalent And Non-Covalent Interfacial Transformations, Ann Fernandez
Behavioral Modulation Of Supramolecular Assemblies Via Covalent And Non-Covalent Interfacial Transformations, Ann Fernandez
Doctoral Dissertations
There are several molecular level mechanisms at the origin of biological functions that serve as inspiration for the development of the “next generation” of materials that display adaptive and interactive properties. However, it will take time for synthetic materials to approach the level of complexity, robustness, and adaptability of biological systems. Although there are switchable platforms that respond via sensitized molecular components, there are currently no examples of materials that truly possess the type of autonomous behavior seen in biological systems. Even though these concepts are common in living organisms, their translation into a synthetic platform remains challenging to this …
Design Of Resposive Oligomeric And Polymeric Interfaces For Sensing And Controlled Release Applications, . Manisha
Doctoral Dissertations
Nature has designed magnificent responsive systems by constructing several interacting molecular level networks for the recognition and propagation of chemical and biochemical information. One of the eminent characteristics of these systems is their capability to quickly transduce molecular scale recognition events into macroscopic or visually observable responses. Inspired by these systems present in nature, we became interested in developing artificial responsive systems with similar capabilities. This dissertation will feature four such systems that employ amphiphilic oligomers and polymers which were chosen as the scaffolds because of their high thermodynamic stability, low critical aggregation concentrations, convenient handles to incorporate functional group …
Engineering Stimuli-Responsive Polymeric Nanoassemblies: Rational Designs For Intracellular Delivery Of Biologics, Kingshuk Dutta
Engineering Stimuli-Responsive Polymeric Nanoassemblies: Rational Designs For Intracellular Delivery Of Biologics, Kingshuk Dutta
Doctoral Dissertations
Biologic drugs have gained enormous research attention in recent years as reflected by the development of multiple candidates to the clinical pipelines and an increased percentage of FDA approval. This is reasoned by the fact that biologics have been proven to deliver more predictive and promising benefits for many hard-to-cure diseases by ‘drugging the undruggable’ targets. However, the challenges associated with biologic drug development are multi-fold, viz, poor encapsulation efficacy, systemic instability, low cellular internalization and endosomal escape capability. Thus, it is essential to develop new molecular strategies that can not only address the associated drug delivery challenges, but also …
Modulating Nanoparticle-Protein Interactions Through Covalent Or Noncovalent Approach For Biomedical Applications, Jingjing Gao
Modulating Nanoparticle-Protein Interactions Through Covalent Or Noncovalent Approach For Biomedical Applications, Jingjing Gao
Doctoral Dissertations
Discoveries at the interface of chemistry, biology, and materials science have emerged as a powerful route to impact life science in this century. My research in the Thayumanavan group is focused on problems at this interface. A common theme of all the six projects is the use of modern synthetic organic chemistry to build interesting, novel macromolecules which are chemically rich, to study the molecular self-assembly behavior in solution and then translate to solve problems in the biomedical area. By addressing the design challenge to prepare novel amphiphiles with desired functional groups, controlled molecular weight and the ability to respond …
Protein Detection And Structural Characterization By Mass Spectrometry Using Supramolecular Assemblies And Small Molecules, Bo Zhao
Doctoral Dissertations
Mass spectrometry (MS) has played an increasingly prominent role in proteomics and structure biology because it shows superior capabilities in identification, quantification and structural characterization of proteins. To realize its full potential in protein analysis, significant progress has been made in developing innovative techniques and reagents that can couple to MS detection. This dissertation demonstrates the use of polymeric supramolecular assemblies for enhanced protein detection in complex biological mixtures by MS. An amphiphilic random co-polymer scaffold is developed to form functional supramolecular assemblies for protein/ peptide enrichment. The influences of charge density and functional group pKa on host-guest interactions …
Providing Molecular Insight For Understanding Anion Exchange Membrane Conductivity, Michael Kwasny
Providing Molecular Insight For Understanding Anion Exchange Membrane Conductivity, Michael Kwasny
Doctoral Dissertations
Anion exchange membranes (AEMs) are notorious for having both low alkaline stability and poor ion conductivity in fuel cell operation conditions, with solutions to these two challenges often being developed independent of each other. The chemical instability of an AEM is viewed through degradation of the polymer backbone and the cationic species and improving a material’s stability is approached by altering the polymer backbone, the cation, or both. On the other hand, poor ion conductivity is typically addressed by modifying bulk membrane properties such as increasing the ion exchange capacity (IEC), changing the morphology, or increasing the water uptake. These …
Reactive And Stimuli-Responsive Sulfonium-Based Polymer Zwitterions, Cristiam Santa Chalarca
Reactive And Stimuli-Responsive Sulfonium-Based Polymer Zwitterions, Cristiam Santa Chalarca
Doctoral Dissertations
This dissertation describes the synthesis and characterization of novel monomers and (co)polymer zwitterions that incorporate trialkylsulfonium cations. The novel materials presented herein constitute a unique type of polymer zwitterions that exhibit salt- and temperature-dependent water solubility as well as inherent reactivity. The behavior of these polymers in aqueous solutions, as nanostructures, and at liquid-liquid interfaces was studied; in all cases, the inherent reactivity of the polymers was harnessed towards the fabrication of novel polymers and soft materials. Following an introductory chapter, Chapter 2 describes the synthesis of sulfonium sulfonate monomers and polymer zwitterions. Both styrenic and methacrylic monomers were synthesized …
Design, Synthesis And Study Of Functional Amphiphilic Polymers And Their Applications, Huan He
Design, Synthesis And Study Of Functional Amphiphilic Polymers And Their Applications, Huan He
Doctoral Dissertations
Amphiphilic homopolymers with high densities of functional groups are synthetically challenging. Thiol-yne nucleophilic click reactions have been investigated to introduce multiple functional groups in polymers with high density. An electron deficient alkyne group bearing methacrylate monomer was polymerized using reversible addition−fragmentation chain-transfer (RAFT) polymerization. Subsequently, the electron deficient alkyne group on polymer side chain was readily reacted with a thiol reagent using triethylamine (TEA) as the organocatalyst. This reaction was found to be very efficient under mild conditions. The resultant homopolymer bearing thiol vinyl ether functional groups could perform a second thiol addition with a stronger base, such as triazabicyclodecene(TBD), …
Modification Of 2d Materials Utilizing Functional Polymer Interfacial Layers, Ryan Selhorst
Modification Of 2d Materials Utilizing Functional Polymer Interfacial Layers, Ryan Selhorst
Doctoral Dissertations
This dissertation describes the modification of 2D transition metal dichalcogenides (TMDCs). These materials exhibit unique electronic properties, ranging from metallic to insulating, and can transport either electrons (n-type) or holes (p-type). Polymers containing electronically-active moieties offer a path to control the electronic properties of a 2D material without altering the inherent structure of the semiconductor. This dissertation focuses on the synthesis of polymers bearing chalcogen-rich or zwitterionic moieties to alter the electronic and solution properties of 2D materials. Chapter 2 describes polymers containing sulfur-rich tetrathiafulvalene (TTF) and their effects as electroactive coatings on the TMDC molybdenum disulfide (MoS2). …
Design And Self-Assembly Of Responsive Scaffolds For Food And Sensing Applications, Uma Sridhar
Design And Self-Assembly Of Responsive Scaffolds For Food And Sensing Applications, Uma Sridhar
Doctoral Dissertations
Developing an understanding of how molecules, materials and complex systems contribute to biological functions is important since the interpretation of such mechanisms paves the way to further the development of materials that replicate natural functions or impart the observed properties to synthetic materials. The self-assembly of stimuli-responsive scaffolds based on micelles, liposomes, hydrogels and thin films has been of considerable interest. These systems need to be endowed with certain design features which influence the self-assembly and the responsiveness of the scaffold when subjected to external stimuli which could be physical, chemical or biological in nature. This kind of insight is …
Amphiphilic Assemblies With Responsive Characteristics At Surfaces And Interfaces, Piyachai Khomein
Amphiphilic Assemblies With Responsive Characteristics At Surfaces And Interfaces, Piyachai Khomein
Doctoral Dissertations
Amphiphilic self-assembly has gained a lot of interest in both academic and industrial fields. Amphiphiles have a unique ability to self-assemble in water, providing a range of nanosized materials of various morphologies. Many efforts have been dedicated to developing responsive amphiphilic assemblies by introducing responsive characteristics into the amphiphile building blocks. Responsive assemblies have been utilized in many promising applications such as targeted drug delivery systems, smart sensors, and electronic devices. Here, we reported four different types of responsive assemblies created via the incorporation of different responsive groups either at the material’s surface or interface. To achieve the responsive characteristics …
Impact Of Chemical Doping On The Thermoelectric Charge Transport Of Organic Semiconductors, Connor J. Boyle
Impact Of Chemical Doping On The Thermoelectric Charge Transport Of Organic Semiconductors, Connor J. Boyle
Doctoral Dissertations
The thermoelectric properties of organic semiconductors allow them to directly convert heat into electricity without the use of moving parts and to directly convert electricity into heat without the use of working fluids. These properties offer opportunities for the generation of electricity from non-conventional or renewable sources of heat and for refrigeration without the risk of leaking harmful working fluids at any length scale down to the nanoscale. Since organic materials are lightweight, flexible, and made from abundant resources, these opportunities could one day become affordable for widespread use and could be expanded to include specialized and otherwise difficult to …
Study Of Self-Assembly And Stimuli Responsive Behavior In Polymeric And Dendritic Amphiphiles, Poornima Rangadurai
Study Of Self-Assembly And Stimuli Responsive Behavior In Polymeric And Dendritic Amphiphiles, Poornima Rangadurai
Doctoral Dissertations
Natural processes are intricately detailed and able to convert molecular-level events into macroscopic or visually observable properties. This is made possible through multiple interactions at the molecular level, signaling due to covalent and non-covalent interactions, and supramolecular networks that rely on dynamic, non-equilibrium structures. Detailing processes in this manner is the current quest for material science research and designing materials for this purpose is usually via a key process known as self-assembly. Self-assembly is a process in which a material with varied components organizes itself into a particular pattern due to various specific inter and intra molecular interactions. By understanding …
Formulation And Characterization Of Lipogels As A Tunable Delivery Scaffold, Celia Homyak
Formulation And Characterization Of Lipogels As A Tunable Delivery Scaffold, Celia Homyak
Doctoral Dissertations
Nanomedicines within the clinic commonly utilize lipid-based scaffolds due to their aqueous assembly and non-covalent dual-guest loading capabilities. Nevertheless, poor stability in vivo and premature guest release remains a challenge with these systems. Polymeric nanomaterials are a popular alternative due to their good stability in vivo with controllable guest release. A caveat to polymeric scaffolds though, is the excess synthetic effort involved for non-covalent dual-drug encapsulation. Benefit lies in harnessing advantages of lipid and polymeric materials via lipid-polymer hybrid scaffold. Such materials have promise due to their dual-encapsulation and dual-stimuli-sensitive characteristics. The need to better understand these materials led us …
Design And Synthesis Of Stimuli-Responsive Polymeric Nanogels Towards Therapeutic Translation, Mallory R. Gordon
Design And Synthesis Of Stimuli-Responsive Polymeric Nanogels Towards Therapeutic Translation, Mallory R. Gordon
Doctoral Dissertations
In the application of delivery of therapeutics, nanostructures of various composition have been employed due to their capacity to act as a host for lipophilic payloads. Advances in the synthetic preparation, size, morphology, and chemical or physical characteristics of polymers have impacted their development and versatility. A detailed understanding of polymeric nanoparticle host-guest properties is crucial to their practical translation to specific delivery applications. Further, these features must be highly tailorable to overcome biological barriers, stably encapsulate their therapeutic contexts, and exhibit payload release selectively in the target environment. In this dissertation, we aim to rationally design polymeric nano-scale assemblies …
Light-Harvesting And Light-Responsive Materials For Optoelectronic And Biological Applications, Youngju Bae
Light-Harvesting And Light-Responsive Materials For Optoelectronic And Biological Applications, Youngju Bae
Doctoral Dissertations
In photodynamic therapy, several critical standards are required of photosensitizers including high singlet oxygen quantum yield, biocompatibility in dark, and long term photochemical stability. In addition, current PDT systems lack active targeting strategies to tumor cells, and instead mainly rely on the natural distribution of PS in the body following injection and application of near-infrared light treatment in the tumor region. This thesis describes a series of BODIPY-based molecules that were designed, synthesized and studied as photosensitizers with high singlet oxygen generation capacity through utilizing the heavy atom effect. Additionally, aqueous solubility and active targeting capability were introduced by photosensitizer …
Nanoparticle As Supramolecular Platform For Delivery And Bioorthogonal Catalysis, Gulen Yesilbag Tonga
Nanoparticle As Supramolecular Platform For Delivery And Bioorthogonal Catalysis, Gulen Yesilbag Tonga
Doctoral Dissertations
Nanoparticles (NPs) are being investigated widely for many applications including imaging, drug delivery, therapeutics, materials, and catalysis due to their unique and tunable physical and chemical properties. Among NPs, gold nanoparticles (AuNPs) have attracted great attention due to ease of synthesis and surface functionalization, inertness of the core, biocompatibility, and functional versatility. Introducing supramolecular chemistry into the nanoparticle-based platforms brings out controllable properties, dynamic self assembly processes, and adjustable performance. My research has focused on the synthesis of AuNPs bearing different surface functionalities and their host-guest interactions with synthetic small molecules or commercially available hydrophobic catalysts for delivery and therapeutic …
Analytical Methods To Support Design And Optimization Of Protein Drug Conjugate: Focusing On Haptoglobin-Hemoglobin Complex As A Drug Carrier, Shengsheng Xu
Doctoral Dissertations
Acquired immunodeficiency syndrome (AIDS) remains one of the most serious public health challenges and a significant cause of mortality for certain populations. Despite the large number of antiretrovirals (mostly nucleotide and nucleoside analogs) developed in the past two decades, the inability of small molecule therapeutics to target HIV reservoirs directly creates a significant obstacle to their effective utilization. Indeed, achieving the desired therapeutic effect in the absence of the effective targeted delivery must rely on dosage escalation, which frequently causes severe toxicity. This problem may be solved by conjugation of antiretroviral agents to endogenous proteins (e.g., hemoglobin haptoglobin complex) that …
Stimuli Responsive Polymeric Nanogels For Hydrophobics & Hydrophilics Delivery, Kishore Raghupathi
Stimuli Responsive Polymeric Nanogels For Hydrophobics & Hydrophilics Delivery, Kishore Raghupathi
Doctoral Dissertations
Stimuli responsive nanoparticles have gained significant interest in the drug delivery research. The essential goal of drug delivery is to improve the efficacy of drugs by increasing their stability and bioavailability. Small molecule hydrophobic drugs face limited bioavailability due to their poor water solubility. Biologic drugs on the other hand, lack bioavailability because of their degradation by various enzymes encountered during blood circulation. For a systemic delivery approach, depending on site of drug action, delivery vehicles must pass through several contrasting micro environments before delivering the cargo selectively at the target site. Therefore, it is essential that a delivery vehicle …
Photolysis Of Triazenylbenzoic Acids For Click Chemistry, Adam Gann
Photolysis Of Triazenylbenzoic Acids For Click Chemistry, Adam Gann
Doctoral Dissertations
Copper catalyzed cycloaddition of terminal alkynes and azides has revolutionized the field of bioconjugate chemistry. Unfortunately, typical copper catalysts are known to disrupt relevant biological systems, so it has become necessary to develop new, copper-free methods that are less cytotoxic. particular interest are "click" probes which can be activated with an outside light source, giving the user spatial and temporal control over the system being investigated. We have developed a method in which an aryl diazonium salt is rapidly generated using photolysis of the triazene functional group, and subsequently coupled with an electron rich aromatic nucleophile to yield an azobenzene. …
Design, Synthesis, And Applications Of Nano-Assemblies Based On Amphiphilic Macromolecules, Hui Wang
Design, Synthesis, And Applications Of Nano-Assemblies Based On Amphiphilic Macromolecules, Hui Wang
Doctoral Dissertations
Recent progress in nanotechnology has been significantly impacting a variety of areas such as utilization in microelectronics, multiphase catalysis, sensing and therapeutics. Our interests are to develop new nanomaterials to understand their structure-property relationships and to utilize them for various applications. In this thesis, we discuss our findings on the design, synthesis and applications of nanomaterials formed by self-assembly of amphiphilic molecules. Micelles are self-assembled nanostructures formed by amphiphilic molecules. They are capable of sequestering hydrophobic guest molecules in an aqueous environment. Other than surfactants, micelles can also be formed by amphiphilic polymers or dendrimers, which are macromolecular surfactants in …
Stimuli Responsive Polymer Self-Assembly And Disassembly, Jiaming Zhuang
Stimuli Responsive Polymer Self-Assembly And Disassembly, Jiaming Zhuang
Doctoral Dissertations
Stimuli responsive polymer assemblies have been long investigated for drug application due to their flexibility for surface functionalization to achieve desired interfacial property and capability of acting as a host for payloads encapsulation. These interfacial and host-guest properties are very critical and need to be customized really depending on nature of cargos and specific delivery application. More importantly, these properties are always desired to be adaptable in different environments. For instance, adjustable interfacial property can facilitate the carrier to overcome a variety of different barriers before it reach the target while changeable host-guest property allows to selectively releasing the payload …
Self-Assembly And Stimuli Responsive Disassembly Of Dendritic And Oligomeric Amphiphiles, Krishna Reddy Raghupathi
Self-Assembly And Stimuli Responsive Disassembly Of Dendritic And Oligomeric Amphiphiles, Krishna Reddy Raghupathi
Doctoral Dissertations
Stimuli response is a fundamental process prevalent in all living systems, where a specific function (response) is generated in the presence of a given environmental cue (stimulus). Engineering materials for this process is often accomplished through another basic process, “self-assembly”. By understanding the key aspects of these processes scientists have developed a broad range of materials for a wide array of applications. This dissertation will primarily focus on developing stimuli responsive nanocarriers based on supramolecular assemblies of amphiphilic dendrimers and oligomers for safe transport and selective release of molecular cargo. Our concurrent goal is to also investigate several parameters which …
Supramolecular Strategies For The Generation Of Nanoparticle Assemblies And Biomolecular Thin Films, Bradley P. Duncan
Supramolecular Strategies For The Generation Of Nanoparticle Assemblies And Biomolecular Thin Films, Bradley P. Duncan
Doctoral Dissertations
The conceptual framework of supramolecular chemistry elucidates a powerful set of strategies for chemists to generate functional nanomaterials based on intermolecular forces. My research focused on tuning the molecular interactions of nanoscale components to create larger structures with enhanced properties. In one approach, I developed and optimized an additive-free, nanoimprint lithography-based methodology to generate stable thin films from a variety of proteins. The generalized process retains intrinsic properties of the protein as demonstrated by selective cellular adhesion. The heat and pressure of the nanoimprinting process induces slight structural reorganization of the peptide side chains to yield highly stable films held …
Inkjet Printing For Biosensing And Security Applications, Brian Creran
Inkjet Printing For Biosensing And Security Applications, Brian Creran
Doctoral Dissertations
The adaptation of inkjet printing technology has recently been used to create controlled high throughput micro- and nano-scaled structures. Coupling this technique with gold nanoparticles in our research has produced new platforms for biosensors, chemical patterning, and anti-counterfeiting applications. In this presentation, we will highlight promising fabrication strategies including the development of test strips for the determination of bacteria in drinking water as well as the use of patterned nanoparticles for security applications.
From Molecular Scale To Mesoscale: Establishing Structural Control Organic Photovoltaics Using Organic Nanoparticles, Timothy S. Gehan
From Molecular Scale To Mesoscale: Establishing Structural Control Organic Photovoltaics Using Organic Nanoparticles, Timothy S. Gehan
Doctoral Dissertations
Organic photovoltaic devices use an active layer of organic materials that absorbs light and creates free charges to generate electricity. Such organic photovoltaics have many desirable properties as the final devices can be very lightweight, thin, flexible, have low manufacturing costs, and be semitransparent. These properties make them particularly advantageous for myriad of applications: e.g., use on non-planar surfaces, as tinted coatings on windows, any use for charging low power devices. One of the biggest problems preventing organic photovoltaics from being commercialized is controlling the packing of the organic materials within the active layer from the molecular scale through the …
Conjugated Polymers In Thermoelectric Composites And Small Molecules For High Light Absorptivity, Murat Tonga
Conjugated Polymers In Thermoelectric Composites And Small Molecules For High Light Absorptivity, Murat Tonga
Doctoral Dissertations
Over the past several decades with increasing of global energy demand, thermoelectric materials have gained considerable attention due to their unique ability to directly convert heat to electricity. In addition to inorganic semiconductors, polymers are potential candidates for high-performance thermoelectric applications due to their intrinsic advantages such as low thermal conductivity, solution processability, and roll-to-roll production, lightweight, and flexible thermoelectric modules. This thesis provides an insight into the emerging field of organic thermoelectrics, more specifically, thermoelectric power generation based on the composites of conducting polymers (MEH-PPV, P3HT and PEDOT:PSS) and carbon nanotubes (SWNT, SWNT-COOH, SWNT-OH and MWNT). A substantial portion …
Photochemical Tools For Fluorescent Labeling Of Endogenous Proteins, Stephen T. Mccarron
Photochemical Tools For Fluorescent Labeling Of Endogenous Proteins, Stephen T. Mccarron
Doctoral Dissertations
The study of the dynamic movements of membrane bound proteins is typically achieved through an exogenously applied fluorescent tag or genetic modification of a receptor of interest to spatiotemporally monitor protein location. Techniques often used for labeling proteins include overexpression of a fluorescent protein such as GFP fused to a target protein or the application of antibodies. These methods benefit from superb specificity towards a receptor of interest, but may impose unforeseen consequences when studying natural protein movements. Thus, it is advantageous to development small, modular probes that would allow for visualization of endogenous membrane bound receptors in a minimally …
Polymer And Fullerene Zwitterions: From Synthesis To Solar Cells, Zachariah A. Page
Polymer And Fullerene Zwitterions: From Synthesis To Solar Cells, Zachariah A. Page
Doctoral Dissertations
This thesis describes the synthesis and applications of hydrophilic conjugated polymers and fullerenes containing dipole-inducing pendent groups. The pendent groups include tertiary amines, sulfobetaine (SB) zwitterions, quaternary ammoniums, and sulfonates, providing solubility in polar solvents. Particular emphasis is placed on zwitterions functalized structures. Suzuki-Miyaura (SM) and Horner-Wadsworth-Emmons (HWE) coupling reactions proved valuable for the preparation of the hydrophilic conjugated polymers, while the Prato reaction afforded the functional fulleropyrrolidines. Ultraviolet photoelectron spectroscopy (UPS) probed the interactions between the hydrophilic conjugated polymers and conductive metal substrates. In particular, UPS revealed that conjugated polymer zwitterions (CPZs) substantially reduce work function (Φ) of metals, …