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Journal of Materials Research and Technology. doi: 10.1016/j.jmrt.2023.09.079
Scientific Reports doi: 10.1038/s41598-023-41947-z
Journal of Chemical Theory and Computation doi: 10.1021/acs.jctc.3c00406
Chem doi: 10.1016/j.chempr.2023.07.020
Proceedings of the 14th International Conference on the Technology of Plasticity - Current Trends in the Technology of Plasticity, 475–485. doi: 10.1007/978-3-031-40920-2_49.
Journal of Chemical Information and Modeling. doi: 10.1021/acs.jcim.3c00835
Protein Science doi: 10.1002/pro.4720
AIP Conference Proceedings. doi: 10.1063/5.0145202
Journal of Materials Research and Technology doi: 10.1016/j.jmrt.2023.06.059
Journal of Medical Devices doi: 10.1115/1.4062492
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy In Chemical Engineering.
DISSERTATION ABSTRACT:
Sepsis is a complicated medical emergency and critically ill patients suffering from infectious diseases are at a high risk for developing and dying from sepsis. According to a recent (2019) cohort study from six United States hospitals, suboptimal care (e.g., delay in antibiotics, inappropriate antibiotic therapy) is responsible for 22.7 % of in-hospital sepsis-associated deaths. In September 2020, the World Health Organization called on the scientific community to develop rapid, effective, and affordable tools to improve diagnosis, surveillance, and treatment of sepsis. Our long-term goal throughout this project is to develop a cyclodextrin (CD) impedimetric tongue that can provide early warning of sepsis by continuous monitoring the course of the disease and real-time profiling of urine samples in hospitalized patients. The cyclodextrin impedimetric tongue will also enable healthcare professionals to closely monitor the patients, predict sensitivity and resistance to therapies, decide about the dose of medications, and develop more effective personalized therapies for septic patients. Cyclodextrins, oligosaccharides with a hydrophobic cavity and a hydrophilic surface, are promising biorecognition elements in development of reusable impedimetric tongues. Cyclodextrins can semi-selectively detect different metabolites in the solutions through hydrophobic interactions, Van der Waals forces, and hydrogen bonding. The first aim of this thesis was to develop the first reusable nanostructured cyclodextrin platform using αCD and a weak surface αCD mediator: polyethylene glycol (PEG). To create the Gold-PEG:αCD surface, gold surface was modified with PEG via thiol-gold chemistry and the PEG support enabled reversible immobilization of αCD. We investigated the performance of this platform for detection of a XVI model hydrophobic analyte, trans-resveratrol. Non-faradaic electrochemical impedance spectroscopy (EIS) measurement of the surface suggested that when αCD surfaces are introduced to a solution containing trans-resveratrol, αCD molecules leave the PEG support to interact with trans-resveratrol in the solution. After use, the surface could be regenerated by reloading of αCD. The second aim of this thesis was to improve the stability and reusability of cyclodextrin sensing platform by replacing gold-thiol bonds with carbon-carbon covalent bonds between glassy carbon (GC) and 4-carboxyphenyl diazonium salt. The GC-carboxyphenyl was modified with polypropylene glycol (PPG) through EDC/NHS chemistry. The PPG surface was then loaded with βCD. We used the GC-carboxyphenyl-PPG:βCD surface for sensitive detection of cortisol in biofluids (i.e., urine and saliva), and demonstrated the successful regeneration and reuse of the GC-carboxyphenyl-PPG:βCD surface for ten times. Finally, we employed sensitive, stable, and reusable cyclodextrin nanostructured surfaces to develop the first-generation cyclodextrin impedimetric tongue for separation and classification of four classes of bioanalytes including creatinine, cortisol, glucose, and fumarate. We applied linear discriminant analysis (LDA) to integrate and map the data, and by using the normalized changes in imaginary capacitance of three cyclodextrin surfaces (γCD at 79 Hz, hydroxypropyl-βCD at 0.25 Hz, and hydroxypropyl-γCD at 63.34 Hz), we achieved the 5-fold cross validation accuracy of 69%. Different methods of data preparation, EIS signal processing, and determining the characteristic frequencies of different analytes and single frequencies of cyclodextrin surfaces affect the accuracy of the impedimetric tongue. By optimizing these parameters, we can improve the performance and accuracy of the impedimetric tongue and apply this device for point of need applications.
Submitted to the University of New Hampshire In Partial Fulfillment of The Requirements for the Degree of Doctor of Philosophy in Chemical Engineering.
DISSERTATION ABSTRACT:
In this dissertation, I developed and investigated gelatin-based microporous injectable hydrogels for the encapsulation of stem cells for multiple applications in cell delivery. Utilizing microgels composed from a mixture of gelatin and modified gelatin, I demonstrated the utility of a dual crosslinking mechanism, which enabled rapid gelation and tissue adhesion with improved cytocompatibility. Mesenchymal stem cells (MSCs) encapsulated in this hydrogel proliferated at a more rapid rate than in a nonporous counterpart, and showed increased immunomodulatory potential. Then, I investigated gelatin microporous hydrogel for the encapsulation of MSCs for bone tissue regeneration. Encapsulated cells more readily differentiated into osteoblasts (i.e. boneforming cells) in the microporous environment observed by morphological changes and quantitative assays. This is believed to be due to enhanced cell spreading and cell-cell communication in the unique 3D environment provided to the cells by the microporous hydrogel. Transcriptomic analysis was performed by mRNA sequencing (RNA-seq) of MSCs encapsulated in the differing 3D microenvironments. Results indicated that the 3D environment influenced the expression of genes that are related to cell adhesions, cell-cell interactions, cytoskeletal organization, and matrix remodeling, in addition to MSC differentiation. Because neuronal development is highly dependent on cell-cell communication, I encapsulated an established neural stem cell line (ReNcell) in gelatin microporous hydrogel to investigate neuronal differentiation in comparison to a nonporous analog. Laminin was chemically conjugated to microgel surfaces, which controlled the organization of encapsulated cells in the hydrogel environment. Cell differentiation was examined by immunofluorescence staining, and JC-1 assay was utilized to examine mitochondrial membrane polarization. The microporous hydrogel xii induced substantially greater cell spreading, morphological changes and cell-cell connections than nonporous hydrogel. The majority of the cells in the microporous hydrogel differentiated into neural lineages, evidenced by immunostaining by MAP2 and GFAP. In summary, this work demonstrates the utility of gelatin microporous injectable hydrogels for applications in in situ cell encapsulation and stem cell delivery for tissue regeneration.
CIRP Annals doi: 10.1016/j.cirp.2023.04.015
Dissertation submitted to the Department of Chemistry and the University of Wyoming in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Nanomaterials are a unique class of materials that exhibit unique chemical and physical properties due to their nanoscale dimensions. These properties make nanomaterials well-suited for use in sensing applications, particularly in the development of electrochemical sensors and biosensors. With a wide range of nanoparticle types available, differing in size, shape, and composition, the applications for nanomaterials in electroanalysis are broad and expanding. In particular, well-ordered nanoparticle arrays are attractive platforms for a variety of analytical applications. However, the fabrication of such arrays is generally challenging due to the difficulty of controlling individual nanoparticle nucleation and growth events. This is where Scanning Electrochemical Cell Microscopy (SECCM) comes in. SECCM is a versatile nanofabrication tool that enables the synthesis of individual nanoparticles of controlled size at precisely defined locations on a sample with high spatial resolution (<100 nm). SECCM allows for the fabrication of ordered nanoparticle arrays where individual nucleation and growth events can be detected and controlled, resulting in nanoparticles of controlled size. One application of this technology is developing electrochemical sensors and biosensors, where gold nanoparticles can be modified with biorecognition elements like thiol compounds to detect specific biomolecules. The ability to fabricate well-ordered nanoparticle arrays with controlled size and position using SECCM makes it an ideal tool for developing such sensing devices, providing a powerful and flexible platform for nanofabrication in electrochemical sensing applications.
Small doi: 10.1002/smll.202300323
Macromolecules doi: 10.1021/acs.macromol.2c02378
Nano LIFE doi: 10.1142/S1793984423300017
Chemical Society Reviews doi: 10.1039/D2CS01011A
Journal of Chemical Education doi: 10.1021/acs.jchemed.2c00922
Korean Journal of Chemical Engineering doi: 10.1007/s11814-022-1293-y
Journal of Chemical Information and Modeling doi: 10.1021/acs.jcim.2c01487
Materials doi: 10.3390/ma16020572
ACS Applied Bio Materials doi: 10.1021/acsabm.2c00910
Journal of the American Chemical Society doi: 10.1021/jacs.2c05510
ACS Nano. doi: 10.1021/acsnano.2c02529
Computer Methods in Applied Mechanics and Engineering. doi: 10.1016/j.cma.2022.115740
ACS Nano doi: 10.1021/acsnano.2c09336
Biofabrication doi: 10.1088/1758-5090/ac94a1
Accounts of Materials Research. doi: 10.1021/accountsmr.2c00173
Current Opinion in Electrochemistry, 37, 101164. doi: 10.1016/j.coelec.2022.101164
Mechanics of Materials. doi: 10.1016/j.mechmat.2022.104480
Book chapter in "Advanced Spectroscopic Methods to Study Biomolecular Structure and Dynamics" doi: 10.1016/B978-0-323-99127-8.00011-8
Ecological Economics doi: 10.1016/j.ecolecon.2022.107624
ASME 2022 17th International Manufacturing Science and Engineering Conference doi: 10.1115/MSEC2022-85595
Environmental Management doi: 10.1007/s00267-022-01715-7
Renewable and Sustainable Energy Reviews doi: 10.1016/j.rser.2022.112898
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
The aim of this dissertation is to provide insight into synthetic materials that replicate the function and structure of natural materials. First, a comprehensive overview of the challenges and recent advances in tailored synthetic molecular recognition through molecularly imprinted polymers (MIPs) will be presented. Chapter 2 of this work discusses the synthesis of azlactonebased homopolymers as functional polymers tuned for the detection of opioid molecules. Through the rapid and efficient ring-opening reaction of azlactone pendant chains with primary amines, customized functionalization of the homopolymers with receptor-like moieties was achieved post-polymerization. Chapter 3 explores the use of functionalized diblock copolymers as protein mimics for single-chain nanoparticle (SCNP) collapse. The collapse was successful by use of a newer, one-pot deprotection and coupling Sonogashira-like reaction without coppercatalyst. The polymers and associated nanoparticles were analyzed by size-exclusion chromatography equipped with a multi-angle light scattering (SEC-MALS) detector. Shifts in retention time from polymer to nanoparticle was indicative of change in hydrodynamic volume, suggesting that the polymer was folded into SCNP. Chapter 4 investigates the use of functionalized diblock copolymers with Diels—Alder reaction compatible monomers to form SCNP. Like Chapter 4, shifts in the retention time were observed between polymer and nanoparticle, and SCNP formation discussed.
Proceedings of the ASEE 2022 Annual Conference. https://peer.asee.org/41107
European Journal of Mechanics - A/Solids, 96, 104775. doi: 10.1016/j.euromechsol.2022.104775
Journal of Medical Devices. doi: 10.1115/1.4055249
Portico. doi: 10.1002/prot.26410
ACS Applied Materials & Interfaces, 14(37), 42374–42387. doi: 10.1021/acsami.2c07701
2022 ASEE Annual Conference & Exposition
International Journal of Computational Materials Science and Engineering doi: 10.1142/S2047684122500154
Journal of Chemical Information and Modeling, 62(14), 3381–3390. doi: 10.1021/acs.jcim.2c00376
Frontiers in Physics doi: 10.3389/fphy.2022.936385
International Journal of Plasticity, 156, 103367. doi: 10.1016/j.ijplas.2022.103367
Journal of Dynamic Behavior of Materials. doi: 10.1007/s40870-022-00344-9
STAR Protocols. doi: 10.1016/j.xpro.2022.101523
Microelectronic Engineering doi: 10.1016/j.mee.2022.111835
IOP Conference Series: Materials Science and Engineering doi: 10.1088/1757-899x/1238/1/012085
Journal of Micro and Nano-Manufacturing doi:10.1115/1.4055474
Proceedings for IISE Annual Conference & Expo 2022
Proceedings of the IISE Annual Conference & Expo 2022.
ACS Applied Bio Materials doi: 10.1021/acsabm.2c00214
Polymer Chemistry doi: 10.1039/D1PY01472B
Proteins: Structure, Function, and Bioinformatics doi: 10.1002/prot.26385
International Journal of Mechanical Sciences doi: 10.1016/j.ijmecsci.2022.107663
CIRP Annals doi: 10.1016/j.cirp.2022.04.059
DISSERTATION ABSTRACT:
Total joint devices that can survive more than 20 years in vivo require a bearing surface that can combine toughness, wear resistance, and chemical stability. Ultrahigh molecular weight polyethylene (UHMWPE) remains the gold standard for these bearings, having been utilized as a liner and bearing surface for over five decades. Well-documented material trade-offs lead to failure modes that suggest that hip liners and knee bearing surfaces without optimal processing may be prone to premature failure in the patient. Because the demographic of those receiving implants is changing and smart materials and devices are seeing increased use in medicine, implants may need to be more functional to allow optimization for the patient of the future. The present work explores material trade-offs by attempting to alter the microstructure of UHMWPE through the use of a severe plastic deformation technique known as equal channel angular pressing (ECAP). Work was performed to confirm the validity and reliability of dynamic mechanical analysis (DMA) as a rapid means to indicate and assess changes to the microstructure of UHMWPE in the form of entanglement density and chain interactions. ECAP was applied to both neat and conductive composites of UHMWPE in order to understand the microstructural and mechanical changes due to shearing. Two grades of UHMWPE were used to understand the impact of MW, a variety of temperatures were employed to better optimize shear strain, and consolidation and extrusion hydrostatic pressures were altered to determine if chain mobility and consolidation were hindered under large compressive forces. Preliminary modeling of the different thermal gradients that ECAP and compression molded (CM) controls are exposed to was carried out to aid in and inform future experiments. While ECAP did not reveal changes to the microstructure of neat materials as compared to compression molded (CM) controls, work-to-failure was decreased which is hypothesized to be due to residual stresses. Carbon composites, on the other hand, were shown to have increased work-to-failure after shearing which was coincident with a decline in conductivity as compared to CM controls.
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Single-chain nanoparticles (SCNP) are a class of intramolecular cross-linked polymeric nanoparticles with a variety of applications including catalysis, sensors, nanomedicine, and nanoreactors. Such nanoparticles are synthesized by folding or collapsing single polymer molecules. By implementing a single-chain folding technique, the single-chain nanoparticles with uniform degrees of cross-linking are synthesized by parent polymer chains with similar chain lengths and polymer microstructure. Polymer chains that are synthesized by various controlled polymerization techniques can be converted to SCNPs through a variety of covalent chemistry and supramolecular interactions. Based on the expected cross-linking chemistry, related functional groups can be installed either during monomer synthesis or post-polymerization functionalization by utilizing a variety of methodologies. With the goal of effecting catalysis of various organic reactions in aqueous system, we developed a series of ligand functionalized SCNPs with water-soluble pendent groups. N-heterocyclic carbene (NHC) ligands were designed and synthesized to immobilize transition metal cation on SCNPs for catalysis. By employing polymer functionalization strategy, amine-ended ligands, water soluble pendent groups, and cross-linkers were installed by substitution reaction on poly xii (pentafluorophenyl acrylate) (PFPA) synthesized by reversible addition fragmentation transfer polymerization (RAFT), and the process of reaction can be monitored by F19 NMR conveniently. Moreover, to realize inverse temperature dependent controlling, the temperature sensitive watersoluble pendent groups were utilized, such as N-isopropyl amide, which can be installed by the addition of isopropylamine in the process of functionalization of poly (PFPA). Consequently, a variety of organic reactions could be possible in aqueous system catalyzed by combination of different transition metal cations and water-soluble NHC-functionalized SCNP platform.
Submitted to the University of New Hampshire In Partial fulfillment of The Requirements for the Degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Certain organisms living in cold regions have adapted different strategies to survive in harshly cold temperatures. Some of them use freeze-avoiding strategies in which they can prevent freezing by controlling the concentration of sugars (et. sucrose, trehalose) or polyols (glycerol), regulation of the ice nucleator, and dehydration. Other organisms have adapted to this extremely cold condition by producing antifreeze (gly)proteins (AF(G)Ps) which exhibit ice recrystallization inhibition (IRI), thermal hysteresis activity (THA), and dynamic ice crystal shaping. These proteins discovered in Antarctic fish in 1960 for the first time have been reported in bacteria, fungi, insects, and plants. AF(G)Ps and their synthetic biomimetics have received increasing attention as potential candidates for various industrial and bio-medical applications. Promising results from vitrification and other protocols using antifreeze agents with ice recrystallization inhibition activity have widely been reported in biopreservation. Conversely, understanding of the antifreezing process caused by these macromolecules remains under challenge. This is due to the multifunctional nature of the freezing process and antifreeze macromolecule’s behavior which brings complexity in designing the synthetic antifreeze structures. In addition, the cost, low availability, toxicity at higher concentrations, and instability beside several other drawbacks make their large-scale production challenging. Although several synthetic attempts for the exploitation of AFPs have been studied in the past, challenges remain in the synthetic design of AFP analogs. On the other hand, poly (vinyl alcohol) (PVA) with simple structure has been reported with potent IRI activity as a good candidate for large-scale production and applications.
Our group has explored structural variations to polyol-based polymers to contrast with PVA as a control and identified several key structural elements for performance in IRI, THA, as well as in ice nucleation inhibition (INI). These structural features are bioinspired by the typical ice-binding plane of AFPs yet are surprisingly simple to produce with potency approaching that of typical AFPs. Key to the performance is positioning small organic functionalities with known antifreeze properties (glycerol) pendent to a host polymer chain with consideration of their conformational freedom. To build systematic variations into both the backbone and side-chain structures, we used poly (vinyl alcohol), poly (isopropenyl acetate), poly (acrylic acid), and poly(methacrylic acid) xvi parent polymers for such pendent modifications. One structure in particular, glycerol-grafted-PVA (G-g-PVA), shows potency rivaling that of AFPs at similar micromolar concentration. The findings in this study help guide the rational design of synthetic antifreeze polymers useful for applications such as anti-icing coatings through to cryopreservation methods for organ transport and cell preservation.
While AFPs are well-known for their ice nucleation and recrystallization inhibition activity along with controlling the ice crystal morphology, the contrasting behavior of ice nucleation promotion by AFPs and its key contribution to the whole antifreezing process also seems necessary to explore in this context. Here, silver iodide (AgI) has been used as an ice nucleator in different polymer solutions in ultra-pure water (UPW) to imitate the ice nucleation process by AFPs. PVA prepared by RAFT polymerization and our glycerol grafted derivative (G-g-PVA), now shown to be the most IRI active polymer to date, was investigated for its ice nucleation and recrystallization activity in AgI dispersion media. The results showed that the ice nucleation rate and temperature was significantly changed by adding the AgI dispersion in PVA and G-g-PVA solutions. The polymer solution in UPW containing AgI dispersion showed significant improvement in IRI activity compared the same polymer in PBS buffer solution. Our results demonstrate the considerable contribution of the ice nucleator in ice nucleation rate and temperature which enhances IRI activity of synthetic antifreeze polymers. These finding both aid our understanding of the ice nucleation promotion impact on synthetic polymers IRI activity along with engineering biomimetics for biomedical and industrial applications.
Next, we focused our efforts to transfer these functionalities and performance to the solid-state interface with water. Aqueous dispersions of polymeric colloidal particles served as this substrate and were functionalized with either PVA or G-g-PVA grafted to their surfaces to contrast with performance of the same polymers strictly in the solution state. These functionalized colloids also can be applied as a continuous coating through latex film formation to assess anti-icing and iceadhesion properties. While these systems also showed encouraging and potent activity, their performance was not enhanced compared to that of the solution state systems. This may have implications for fully solid-state anti-icing coatings, yet our attention then shifted from this scope of work to new funding which required again a solution state approach.
In this final application, we explored PVA and G-g-PVA synthesized in our lab for their biopreservation aspects especially for red blood cell (RBC) cryopreservation at -80 °C. Our results again confirmed G-g-PVA to be an excellent candidate for cryopreservation and quite likely for organ cryopreservation. Using this polymer in solution as a cryoprotectant for RBCs showed significant improvement to controls, preventing hemolysis (cell rupture) along with eliminating other drawbacks that have been observed when using small molecule cryoprotective agents like glycerol, dimethyl sulfoxide (DMSO), etc.; especially with regard to the ability to fully remove all traces of the cryoprotectant after cryopreservation storage and thawing.
In summary, the studies in this dissertation provide critical insights and approaches for the understanding of the freezing process and ideas that can help understand relevant mechanisms of influencing key freezing steps that have not yet been fully understood. In addition, it provides guidelines to synthesize G-g-PVA, currently the most potent active polymer in terms of IRI and THA shown useful for several high impact applications. In particular, this research provides valuable data and experimental conditions to understand the IRI mechanism to use in engineering next generation highly efficient antifreeze systems.
Submitted to the University of New Hampshire In Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy In Chemical Engineering.
DISSERTATION ABSTRACT:
In this dissertation I investigated the structural properties of melanin biopigment from different sources as an antibacterial and endotoxin bonding agent. I extracted melanin from Equus ferus hair with acid hydrolysis (termed EquusMel) and characterized it by microscopic and spectroscopic techniques. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) revealed that EquusMel is mainly elliptical in shape with a mesoporous and layered structure within the individual particles. Wide-angle (WAXS) and small-angle (SAXS) Xray scattering measurements demonstrated a semicrystalline multilayered structure with order spacing of 45.2 Å. Pore size distribution determined by the Barrett–Joyner–Halenda (BJH) method showed primary pores within the range of 30–50 Å. Nitrogen adsorption–desorption isotherms exhibited a Brunaur–Emmett–Teller (BET) surface area of 3 m2 /g. Raman, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR) spectra revealed similar chemical signature between EquusMel and synthetic melanin (SynMel). I investigated the antibacterial effect and its mechanism of action for EquusMel. I found that EquusMel has distinct antibacterial activity due to its potential to generate reactive oxygen species (ROS). ROS generated via oxidation of catechols is considered the main mechanism of antibacterial activity. The simplicity of EquusMel extraction and its antibacterial property allows this biomaterial to be xvi applicable to a variety of areas. Zinc cations (Zn2+) were loaded on melanin structure (Mel-Zn) for rapid and selective separation of gram-negative bacteria and lipopolysaccharide (LPS) from blood. Mel-Zn was characterized by XPS and Raman which revealed the successful Zn2+ loading. I identified that Mel-Zn rapidly captures approximately 90% of Escherichia coli in whole blood and 100% of LPS in PBS, which can reduce bacteremia loads and mitigate the spread of these infectious agents to other tissues and organs. Additionally, simultaneous binding to bacteria and LPS could enhance the efficacy of antibiotic therapy. Adsorption of protein from individual protein model solutions, as well as LPS-spiked protein solutions, was found to be minimal. Hemolysis and coagulation assays demonstrate the blood biocompatibility of Mel-Zn, which could be adapted for clinical use in an extracorporeal membrane to remove pathogens and LPS in acute sepsis patients.
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Master of Science in Chemistry.
THESIS ABSTRACT:
Understanding the properties of bioconjugates and biomaterials has increasingly become the focus of pharmaceutical companies, material scientists, and academia due to their growing list of applications. Bioconjugates have found broad use in therapeutics, drug delivery, tissue engineering, and biosensing. Historically, interest in specific bioconjugates has depended on the cost-availability of the biomacromolecule, making proteins the most well studied, given their relatively low cost and ease of production. However, recent technological advances in plasmid DNA (pDNA) production from E. Coli allow for greater cost-efficiency, changing the landscape ofbiomaterial research. Employing alkylating agents with known chemo-selectivity to nucleophilic sites on DNA, a polymer or polymerization agent can be coupled to biologically derived pDNA. Subsequently, properties of the hybrid-DNA bioconjugate can be controlled via the location of alkylation, to tune degradation rate and stability of the DNA bioconjugate and graft-from polymerization to increase stability and solubility.
Submitted to the University of New Hampshire in Patrial Fulfillment of the Requirements of the Degree of Master of Science in Mechanical Engineering.
THESIS ABSTRACT:
In-plane biaxial testing using a cruciform type specimen is a useful experimental method to characterize the elasto-plastic material behavior under non-uniaxial conditions. Different stress states can be imposed to the specimen simply by varying loading ratios along two orthogonal axes. Experiments can be performed using one experimental setup and one specimen geometry. Among different control options for loading, the displacement control in each arm is a stable and consistent option to keep the static deformation rate. However, a non-linear relationship exists between the control parameter e.g., displacement, and derived quantities, e.g., stress and strain. Therefore, it is a challenge to achieve desired deformation paths in the main deformation area of the specimen. In this document, an interpolation method to systematically determine nonlinear displacement paths is implemented using the finite element simulation method to produce linear stress and strain paths in the center of a cruciform specimen geometry. Interpolation is first applied to an AISI 1008 steel specimen, in which a previously interpolated linear strain path is improved with another iteration of interpolation. Interpolation is then expanded to produce displacement paths resulting in linear stress paths, having a constant stress triaxiality, for five different stress states of a SS304L cruciform specimen. The versatility of the interpolation method is displayed through the successful implementation for both strain and stress linearization as well as with two different materials and two specimen geometries.
Drones doi: 10.3390/drones6050100
Computational Materials Science doi: 10.1016/j.commatsci.2022.111348
Journal of Micro and Nano-Manufacturing doi: 10.1115/1.4055230
Mahmud, M.S. (2022) "Healthcare data analytics for wearable sensors". In E.M. Narvaez, C. Dincer (Ed.). Wearable Physical, Chemical and Biological Sensors: Fundamentals, Materials and Applications (pages 169-182). Elsevier. doi: 10.1016/c2019-0-04003-4
Cell Reports Physical Science doi: 10.1016/j.xcrp.2022.100786
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Journal of Applied Polymer Science doi: 10.1002/app.52175
ACS Applied Polymer Materials. doi: 10.1021/acsapm.1c01312
International Journal of Molecular Sciences. doi: 10.3390/ijms222413481
Polymer Chemistry. doi: 10.1039/D1PY01005K
ACS Applied Materials & Interfaces doi: 10.1021/acsami.1c14453
ACS Applied Materials & Interfaces. doi: 10.1021/acsami.1c14453
Angewandte Chemie International Edition. doi: 10.1002/anie.202113665
Chemical Society Reviews doi: 10.1039/d1cs00600b
Chemical Society Reviews. doi 10.1039/d1cs00600b
Angewandte Chemie International Edition. doi: 10.1002/anie.202113569
DISSERTATION ABSTRACT:
Metal–Organic Frameworks (MOFs) and Covalent Organic Frameworks (COFs) are emerging materials with multifunctional properties that allow them to address global issues in chemical separations and sequestration, chemical sensing, and energy storage and conversion. Many of these applications rely on the ensemble of host–guest interactions between targeted molecular species and the surface of the framework to imbue selective properties that enhance applied performance metrics. Design principles guiding the construction of materials with desired surface chemistry and functionality are lacking for framework materials targeted towards chemical sensing. A better fundamental understanding of how host–guest interactions inform function and how host sites can be designed into a framework system through bottom-up synthetic techniques is required to advance the field of framework materials for electroanalysis. In four chapters, this thesis provides insight into the role of surface chemistry in chemical sensing in both the liquid and gas phase and how the interplay between surface chemistry and conductivity can be controlled by the strategic choice of starting materials and material morphology to produce materials with robust capabilities in chemicals sensing.
Frontiers in Chemistry. doi: 10.3389/fchem.2021.753635
Biophysical Journal. doi: 10.1016/j.bpj.2021.10.007
International Journal of Computational Materials Science and Engineering. doi: 10.1142/s2047684121500329
Frontiers in Physics. doi: 10.3389/fphy.2021.767623.
Proteins. doi: 10.1002/prot.26265
Physical Chemistry Chemical Physics. doi: 10.1039/d1cp03822b
Sensors and Actuators Reports. doi: 10.1016/j.snr.2021.100051.
Submitted to the faculty in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Designing 3D printable supramolecular materials that can amplify molecular level functions to macroscale promotes the construction of advanced architectures with superior properties, thus accelerating the development of stimuli-responsive materials into integrated devices. Cyclodextrin-based poly(pseudo)rotaxanes, referred to as polyrotaxanes and polypseudorotaxanes, are ideal candidates to exercise the designing principles of 3D printable mechanically interlocked molecules (MIMs) for functional materials, due to their facile synthetic methods, variable stimuli responsiveness, and excellent biocompatibility. In this thesis, I set out to design 3D-printable cyclodextrin-based poly(pseudo)rotaxanes with their molecular motions synchronized to be amplified at the macroscale, subsequently exploiting designed macroscopic shapes with complex structures to advance their macroscopic machinery behaviors.
First, I identified designing principles to facilitate the 3D printability of MIMs for direct ink writing: (1) tailoring the dynamic interactions between binding motifs, such as hydrogen bonding between cyclodextrins, to allow the shear-thinning and rapid self-healing properties; (2) controlling assembled architectures to reinforce the polymer networks. By synthetically navigating the crystalline inclusion complexes to amorphous products with higher crosslinking degrees via the design of speed bumps or side-chain architectures, crystalline precipitates were converted to viscoelastic hydrogels that are favorable for 3D printing and mechanical adaptability. These insights allow us to design a series of 3D-printable cyclodextrin-based poly(pseudo)rotaxanes with controllable network structures and superior mechanical and responsive properties.
Second, I have also demonstrated an approach to synchronize the molecular motions of the mechanically interlocked rings and amplify them to perform mechanical work by switching the motions of the rings between random shuttling and stationary states through different external stimuli. This allows us to develop a family of actuators or mechanically adaptive materials that respond to solvent, pH, temperature, humidity and cyclodextrins, in which their macroscopic motions and materials properties rely on the control of molecular motions or features and hierarchical control across nano-to-macroscale.
Another interesting class of polyrotaxane materials I discovered are anti-freezing hydrogels with excellent mechanical properties. By noncovalently connecting polyrotaxane and polyacrylamide via hydrogen bonds, the resultant pseudo-slide-ring network hydrogels possess high stretchability, high toughness, good electrical conductivity at sub-zero temperatures, paving the way for a wide range of hydrogel applications under extreme environments.
Journal of Alloys and Compounds. doi: 10.1016/j.jallcom.2021.161871.
Fisheries Management & Ecology doi: 10.1111/fme.12513
Journal of Applied Ecology doi: 10.1111/1365-2664.14009
Materials Horizons. doi: 10.1039/d1mh01108a.
Canadian Journal of Fisheries and Aquatic Sciences doi: 10.1139/cjfas-2020-0402
Angewandte Chemie International Edition. doi: 10.1002/anie.202109987
Materials Science and Engineering: A. doi: 10.1016/j.msea.2021.141876
Volume 1: Additive Manufacturing; Advanced Materials Manufacturing; Biomanufacturing; Life Cycle Engineering; Manufacturing Equipment and Automation. doi: 10.1115/msec2021-63658
Volume 1: Additive Manufacturing; Advanced Materials Manufacturing; Biomanufacturing; Life Cycle Engineering; Manufacturing Equipment and Automation. doi: 10.1115/msec2021-63471
Volume 2: Manufacturing Processes; Manufacturing Systems; Nano/Micro/Meso Manufacturing; Quality and Reliability. doi: 10.1115/MSEC2021-59877.
Proceedings of the 2021 IISE Annual Virtual Conference.
The 12th International Conference on Computational Methods.
Forming the Future. doi: 10.1007/978-3-030-75381-8_155
Forming the Future. doi: 10.1007/978-3-030-75381-8_166
Chem. doi: 10.1016/j.chempr.2021.06.004
JOM. doi: 10.1007/s11837-021-04715-w
JOM. doi: 10.1007/s11837-021-04715-w
Journal of Manufacturing Science and Engineering. doi: 10.1115/1.4051189
CIRP Journal of Manufacturing Science and Technology. doi: 10.1016/j.cirpj.2021.04.006
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Given the rising of environmental concern, the market of waterborne coating and adhesives has been constantly growing. Polymer latex particles produced by emulsion polymerization are one type of important components in their formulations. Thus, to tune mechanical properties of waterborne coatings and adhesives, one of the common ways is to utilize crosslinkers to form a macromolecular network structure, as known as “gel”, inside of the polymer latex. A major challenge to obtain desired properties of the material is how to control macromolecular architecture, such as sol-gel ratio and crosslinking density. Hence, this dissertation focuses on the study of predicting and controlling macromolecular network architectures in both bulk polymerization and emulsion polymerization. Bulk polymerizations share some similar mechanisms with emulsion polymerization but is simplified by being a homogeneous single phase reaction environment. Emulsion polymerization is a heterogeneous reaction environment with reactions in two phases. Due to the complexity of the emulsion polymerization environment, bulk polymerization is often used xxii as a first test environment to simplify and study new reaction systems. Based on our previous work, a reduced reactivity parameter, Ψ, was introduced and applied to precisely describe the reactivity of crosslinking sites (pendent vinyl groups from crosslinker monomers). Most of our prior work used the bulk polymerization environment and here we now also extend to the emulsion polymerization environment. In addition to crosslinking reaction kinetics, we also explored macromolecular structure development as predicted by a hybrid Monte Carlo Model. Chapter 3 and Chapter 4 significantly extended our previous work. Chapter 3 explored a wide matrix of monomer-crosslinker pairs of varied molecular size and revealed a stronger understanding of the relationship between resulting Ψ values and the structures of each monomer-crosslinker pair. In Chapter 4, another mechanistic factor, reactivity ratio between the crosslinker and the main monomer, was also introduced. This chapter studied how both contributions, Ψ and reactivity ratio, influence the eventual crosslinking reaction. All polymerizations were conducted via bulk polymerization in Chapter 3 and Chapter 4. Emulsion polymerization is a heterophase polymerization and their polymers are known as “products by process”. Here, we fed the monomer mixture to the reaction in a semi-batch mode, and therefore, Chapter 5 mainly studied the influence of the monomer feeding profile on gel formation during emulsion polymerization. A relationship was observed that higher feeding rate can cause higher gel content. This was found to be explained by the dominance of a “micro loop” formation, an intramolecular first order reaction between the chain end radical and its own pendent vinyl group, when the unreacted free monomer concentration was very low (i.e. with slow monomer feed rate to the reactor). These microloops consumed pendent vinyls without allowing a crosslinking event to occur. At higher monomer feed rate, the mechanisms xxiii would start to favor the Ψ and reactivity ratio effects again. This was an important learning on the balance between favored mechanisms as a function of the polymerization process and environment. Chapter 6 is a side but still relevant topic. In this chapter, four different bio-based reactive surfactants were successfully synthesized. They could be used as stabilizers for emulsion polymerization. Two of four of reactive surfactants were two different types of bi-functional surfactants (divinyls, thus also considered crosslinkers). They were proved to not only be able to stabilize the particles, but also be able to crosslink the particles under certain conditions. Chapter 6 is a proof-of-concept study and should not be considered completed work. Nonetheless, it shows great promise for continuation by another student.
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Mechanical Engineering.
DISSERTATION ABSTRACT:
3D woven carbon/epoxy composites are high-performance materials with superior thermomechanical and physical properties making them an integral part of the aerospace, energy and automotive industries. However, under certain manufacturing conditions, these composites may accumulate severe intrinsic manufacturing-induced residual stresses which can even lead to microcracking. The complex reinforcement architecture makes analytical, numerical and experimental analysis of these composites challenging. This research has been focused on micromechanical analysis, computational modeling, and experimental characterization of 3D woven carbon/epoxy composites aiming to evaluate the manufacturing-induced residual stresses and enable mitigation of their negative impact on the resulting performance. A procedure to develop high-fidelity meso-scale finite element models with as-woven representation of the composite reinforcement informed by the μCT scanning was proposed. A set of meso-scale models for different reinforcement architectures was produced and utilized to predict the accumulation of intrinsic manufacturing-induced residual stresses in these composites. The models were correlated to the blind hole drilling experiments and used for interpretation of the experimental results providing full-field spatial distribution of the residual stresses accumulated in the composite specimens. A new simplified approach to account for nonlinear effects in the material due to severe residual stresses using linearly-elastic models was proposed. A set of parametric numerical studies was performed to improve correlation of the models with the experimental measurements. The developed meso-scale models were used to predict effective coefficients of thermal expansion for the composites with temperature-dependent properties of the constituents. Methods presented in this work provide valuable tools for the field of computational and experimental mechanics of textile composite materials.
Physical Chemistry Chemical Physics. doi: 10.1039/d1cp00679g
The Journal of Physical Chemistry B. doi: 10.1021/acs.jpcb.0c11096
Computer Methods in Applied Mechanics and Engineering. doi: 10.1016/j.cma.2021.113747
Environmental Development, 37, 100602. doi:10.1016/j.envdev.2020.100602
Materials Science and Engineering: A. doi: 10.1016/j.msea.2021.140980
Sustainability Science doi: 10.1007/s11625-021-00904-3
Angewandte Chemie International Edition. doi: 10.1002/anie.202017019
Journal of Chemical Theory and Computation. doi: 10.1021/acs.jctc.0c01199
ASME 2020 International Mechanical Engineering Congress and Exposition. doi: 10.1115/imece2020-24111
Journal of Materials Science & Technology, doi: 10.1016/j.jmst.2020.12.047
Proceedings of the ASME 2020 15th International Manufacturing Science and Engineering Conference. Volume 2: Manufacturing Processes; Manufacturing Systems; Nano/Micro/Meso Manufacturing; Quality and Reliability. September 3, 2020. V002T08A012. ASME. doi:10.1115/MSEC2020-8372
Biophysical Journal, doi: 10.1016/j.bpj.2020.12.010
Journal of Micro and Nano-Manufacturing, doi: 10.1115/1.4049364
Journal of the American Chemical Society, doi: 10.1021/jacs.0c07041
Mechanics of Materials, 154, 103707. doi: 10.1016/j.mechmat.2020.103707
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2514738140
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2490074300
ACS Macro Letters, 9, 1836-1843. doi: 10.1021/acsmacrolett.0c00774
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Master of Science in Mechanical Engineering.
THESIS ABSTRACT:
Results for SS316L microtube experiments under combined inflation and axial loading for single and multi-loading segment deformation paths are presented along with a plasticity model to predict the associated stress and strain paths. The microtube inflation/tension machine, utilized for these experiments, creates biaxial stress states by applying axial tension or compression and internal pressure simultaneously. Two types of loading paths are considered in this paper, proportional (where a single loading path with a given axial:hoop stress ratio is followed) and corner (where an initial pure loading segment, i.e., axial or hoop, is followed by a secondary loading segment in the transverse direction, i.e., either hoop or axial, respectively). The experiments are designed to produce the same final strain state under different deformation paths, resulting in different final stress states. This difference in stress state can affect the material properties of the final part, which can be varied for the intended application, e.g., biomedical hardware, while maintaining the desired geometry. The experiments are replicated in a reasonable way by a material model that combines the Hill 1948 anisotropic yield function and the Hockett-Sherby hardening law. Discussion of the ix grain size effects during microforming impacting the ability to achieve consistent deformation path results is included.
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Master of Science in Mechanical Engineering.
THESIS ABSTRACT:
This work presents improvements to the methods used in crystal plasticity simulations. It shows how these improvements can be used to accurately predict the deformation behavior of two magnesium alloys, WE43, and AZ31. The first improvement to the methodology is guidance on the type of finite elements to use in explicit grain crystal plasticity simulations. This study found that quadratic tetrahedral and linear hexahedral elements are the most accurate element types included in the study. The study also concluded that tetrahedral elements are more desirable due to fast mesh generation and flexibility to describe geometries of grain structures. The second improvement made was the addition of a numerical scheme to enable the use of any rate sensitivity exponent in the fundamental power-law representation of the flow rule in crystal visco-plasticity. While allowing the use of even very large exponents that many materials exhibit, this numerical scheme adds little to no increase in computational time. This crystal plasticity model was used to accurately predict the deformation behavior of both WE43 and AZ31 under quasi-static and high rate deformation, predicting the stress-stain response and the evolution of texture, twinning and the relative activities of the various deformation modes.
Journal of Materials Chemistry B, doi: 10.1039/d0tb02475a
Elementa: Science of the Anthropocene, 8(1). doi:10.1525/elementa.003
Elementa: Science of the Anthropocene doi: 10.1525/elementa.003
Energy Policy, 143, 111457. doi:10.1016/j.enpol.2020.111457
Materials Science and Engineering: A. doi: 10.1016/j.msea.2020.140478
Environmental Research Letters, 15(10), 104054. doi:10.1088/1748-9326/abad58
Journal of Molecular Biology. doi: 10.1016/j.jmb.2020.08.026
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2445953572
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2445435236
Soft Matter, 16, 8101-8107. doi: 10.1039/d0sm00954g
Entropy, 22(8), 877. doi:10.3390/e22080877
International Journal of Plasticity, 136, 102807. doi: 10.1016/j.ijplas.2020.102807
Chemistry of Materials. doi: 10.1021/acs.chemmater.0c01007
Nano Research. doi: 10.1007/s12274-020-2874-x
Restoration Ecology. doi:10.1111/rec.13228
Restoration Ecology doi: 10.1111/rec.13228
UNH Scholars Repository (Carsey School of Public Policy)
Resources, Conservation and Recycling, 161, 104990. doi:10.1016/j.resconrec.2020.104990
The Journal of Physical Chemistry Letters. doi:10.1021/acs.jpclett.0c01390
Chemistry of Materials. doi: 10.1021/acs.chemmater.9b05289
Memorandum prepared for the U. S. Fish and Wildlife Service, Coastal and Partners Program. Brett Still and Art Gold facilitated URI support for this publication and 7 Future of Dams graduate students were recognized for their assistance with field work, data management and processing, and GIS mapping.
Acta Materialia, 195, 59-70. doi: 10.1016/j.actamat.2020.04.036
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2439345330
Submitted to the University of New Hampshire In Partial Fulfillment of the Requirements for the Degree of Master of Science In Chemistry May 2020.
THESIS ABSTRACT:
This thesis explores the use of Diels-Alder functionalized particles to aide in the mechanical enhancement of additively manufactured objects. To date, materials generated via additive manufacturing lack isotropic properties due to the nature in which they are created – in a layer by layer fashion. This methodology often leads to poor interfacial adhesion at the junction between printed layers, lowering the stability of the part and thereby limiting its use in many applications. Dynamic covalent chemistry, such as the reversible Diels-Alder reaction, has the ability to alleviate this anisotropy to print stronger, more uniform objects. To do so, this work investigates crosslinked, Diels-Alder functionalized particles generated by two separate methods: polymerization via reversible addition fragmentation chain transfer (RAFT) followed by atom transfer radical coupling (ATRC) and free radical emulsion polymerization. These particles can be blended with a polymeric filament for 3D printing, where upon heating during the extrusion process of additive manufacturing, the retro-Diels-Alder reaction is initiated and releases the crosslinked particles exposing reactive diene and dienophile pairs. In subsequent xvii cooling after the printing process, these moieties undergo the forward Diels-Alder reaction and form chemical linkages between printed layers of the substrate to improve the mechanical integrity and uniformity of objects produced by means of additive manufacturing.
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2444866135
UNH Scholars Repository https://scholars.unh.edu/cgi/viewcontent.cgi?article=1012
ProQuest Dissertation or Thesis https://www.proquest.com/docview/2434061589
Submitted to the Faculty in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Since the discovery of electrically conductive two-dimensional (2D) metal–organic frameworks (MOFs), the synthetically tunable properties and intrinsic porosity of these materials make them promising for multifunctional sensing devices. The focus of my work is on a class of 2D MOFs based on a triphenylene core (2,3,6,7,10,11- hexahydroxytriphenylene, HHTP and 2,3,6,7,10,11-hexaiminotriphenylene, HITP) coordinating to divalent Cu or Ni metal nodes forming M3HXTP2 MOF analogs (M = Ni, Cu; X = NH, HITP or O, HHTP). Chapter 2 describes a simple strategy for device fabrication, using mechanical abrasion, enabling the chemiresistive sensing of NH3, H2S, and NO. The value in this contribution is threefold. First, the technique may be applicable to a wide range of materials, both semiconductors and possibly insulators. Second, the rapid prototyping method enables direct deposition using mechanical abrasion on a wide range of substrates. Third, the integration of the MOF-based sensing material into devices is entirely solvent-free, which can preserve device substrates sensitive to harsh solvents. Chapter 3 describes a new strategy of MOF synthesis termed oxidative restructuring that feature several innovative characteristics that advance the field of MOF integration. First, oxidative restructuring enables the facile integration of Cu3HHTP2 and Cu-BTC onto prepatterned Cu layer on multiple substrates. Second, we detail spectroscopic evidence that provides insight into the interaction between Cu3HHTP2 and NO using diffuse reflectance infrared fourier transform spectroscopy and X-ray photoelectron spectroscopy. Third, Cu3HHTP2 MOF devices demonstrated the highest dynamic loading capacity of NO and functioned as chemiresistive sensors for the detection of NO and H2S. Chapter 4 describes the implementation of 2D MOF based electrodes to enable the voltammetric detection of biologically relevant analytes. First, strategic selection of redox active analytes combined with the electrochemical methods, allowed us to investigate the intrinsic electrochemical properties of M3HXTP2 MOF analogs (M = Ni, Cu; X = NH, HITP or O, HHTP). Second, this demonstrated one of the first uses of 2D MOFs in solution phase detection with nanomolar detection at 63 ± 11 nM for dopamine and 40 ± 17 nM for serotonin. Taken together, chapters 1-4 advance the field of conductive metal–organic frameworks by providing insight in molecular engineering of MOFs that guides the iii structure property relationships to enable precise function for chemical detection and provides strategies for the strategic integration of MOFs on substrates.
Journal of the American Chemical Society. doi: 10.1021/jacs.9b13402
Chemistry of Materials. doi: 10.1021/acs.chemmater.9b04092
PLOS ONE, 15(3), e0229501. doi:10.1371/journal.pone.0229501
Authorea doi: 10.1002/essoar.10502249.1
Poroi, 12(1). doi:10.13008/2151-2957.1302
Environmental Sociology, 1–13. doi:10.1080/23251042.2019.1696008
Soft Matter. doi:10.1039/c9sm01878f
Environmental Communication, 14(3), 416–429. doi:10.1080/17524032.2019.1686408
In Developing Change Agents Edited by Kristi L. Kremers, Alexander S. Liepins, and Abigail M. York. EBOOK ISBN: 978-1-946135-57-5
Polymer Chemistry. doi:10.1039/c9py01510h
Stochastic Environmental Research and Risk Assessment. doi: 10.1007/s00477-019-01726-7
Submitted to the University of New Hampshire in Partial Fulfillment of the Requirements for the Degree of Master of Science in Mechanical Engineering September, 2019.
THESIS ABSTRACT:
The following research explores the continuous bending under tension (CBT) incremental forming process effects on four dual phase (DP) steels: DP 590, DP 780, DP 980, DP 1180. A parameter study was conducted, finding the ideal parameters for increased elongation to fracture compared to tension of over five times for DP 1180 and DP 980. These parameters were found to be a normalized bend depth of 3.5 and a crosshead pull speed of 1.35mm/s. Using these parameters, following tests were conducted on all four steels by stopping the CBT process before fracture at 2, 4, 6, 8, and some even at 10 and 12 CBT cycles. Smaller tensile specimens were machine from these CBT processed strips and uniaxial tension tests were performed to study the residual ductility of CBT testing. The strength of all steels increased with increased cycle count by 200-400 MPa, however the ductility decreased by over half. Using neutron diffraction, the texture evolution of the CBT process was explored. Results showed a preferred orientation in the {011} fiber in the pulling direction. This research also proves simulating the CBT process and matching to experimental data can be a method for extrapolating post-necking hardening behavior of DP 980 and DP 1180. The experimental data and results are further explained in the following chapters.
Physical Chemistry Chemical Physics, 2019. doi: 10.1039/c9cp04408f
Nat Sustain 2, 647–649 (2019) doi:10.1038/s41893-019-0357-4
Many of New Hampshire’s dams are reaching the end of their lifespan and require expensive maintenance or removal in order to meet safety standards. While engineers and public officials struggle with the scale of the challenge surrounding various dam management alternatives, including removal, what does the New Hampshire public think? In this brief, authors Natallia Leuchanka, Catherine Ashcraft, Kevin Gardner, and Lawrence Hamilton present results from statewide surveys in New Hampshire that explore public views about dam removal. They report that a majority of respondents in three Granite State Polls prefer to remove dams when the alternative is to keep them for maintenance of waterfront property values, preservation of industrial history, or maintenance of lake- and pond-based recreation. A majority of survey respondents prefer to keep dams when dams are for hydropower generation. Respondents’ age, gender, and party affiliation often predict their preference for dam removal. Levels of formal education do not make much difference. Younger respondents, women, and Democrats are more likely to support dam removal, although this varies somewhat depending on the tradeoffs.
North American Journal of Fisheries Management, 39(5), 989–998. doi:10.1002/nafm.10330
Molecular Simulation, 45(14-15), 1273–1284. doi: 10.1080/08927022.2019.1634268
Journal of the American Chemical Society 2019 141 (30), 11929-11937. doi: 10.1021/jacs.9b03441
Science of The Total Environment, 669, 833–843. doi: 10.1016/j.scitotenv.2019.03.042
Sustainability Science. doi:10.1007/s11625-019-00707-7
International Journal of Solids and Structures, 174-175, 28–37. doi: 10.1016/j.ijsolstr.2019.06.005
Chemistry – A European Journal, 25(46), 10768–10781. doi: 10.1002/chem.201900975
This dissertation has been examined and approved in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemistry.
DISSERTATION ABSTRACT:
Atom transfer radical coupling (ATRC) is gaining recognition for its utility in building complex polymeric architectures because it features efficiency, a wide range of compatible substrates, and a lack of byproducts. These qualities are especially desirable in applications requiring intramolecular cross-linking as in the synthesis single-chain nanoparticles (SCNP). This dissertation aims to (I) provide motivation and context for developing ATRC technology for intramolecular cross-linking, (II) provide guidance into the impact of catalyst selection and substrate on reaction efficiency and morphology, and (III) demonstrate the possibility to sequence intrachain ATRC with ATRP to create advanced SCNP architectures. Chapter II describes the preparation of SCNP from parent polymers containing alkyl or benzyl bromide ester pendants using ATRC catalyzed by copper halides complexes. Tri- or tetradentate alkyl or pyridyl amines (PMDETA, TPEN, and TPMA), which tune the redox potential of the Cu(I)/Cu(II) system, were directly compared. Coupling efficiency was positively correlated with the kATRP of the respective catalyst systems. However, PMDETA complexes afforded greater control as evidenced by lower polydispersity. In the case of alkyl halide pendants, selectivity for coupling over disproportionation systematically decreased under conditions designed to increase the concentration of CuI /L. Polymers with benzyl bromide pendants, which cannot disproportionate, tended to produce high molecular weight products, even in ultradilute solutions (0.25 –1.0 mg/mL). xvii Chapter III describes the preparation of SCNP from parent polymers capable of initiating intra-chain polymerization by ATRP under conditions favoring termination by coupling. Because of the wide variety of compatible monomers that have been well-established for ATRP systems, the ATRP/C framework both simplifies reaction procedures (one pot polymerization and coupling strategies are feasible) and imparts handles with which to control both architecture and functionality. To demonstrate this potential, model simple brushes and hyperbranched examples were prepared. SCNP with the hyperbranched motif were remarkably dense, a result which demonstrates the potential to facilitate more globular SCNP structures using modifications of intrachain polymerizations. Methacrylic brush arms, which are not non-ATRC active, could be induced to couple by adding 5 equivalents of styrene under the shared ATRP/C conditions. In addition, it was determined that hyperbranched SCNP retain “living” ω-ends which may be initiated to perform post-collapse polymerizations. A model styrene example is presented; despite occurring in an ultradilute solution, the polymerization maintains fidelity to pseudo-first order kinetics. In sum, there is currently a great impetus for pushing the boundaries of structural and functional complexity that can be designed using the single-chain nanoparticle motif. Atom transfer radical chemistry is a particularly versatile example and it is my hope that this work facilitates the creation of new creative and functional designs.
Journal of the American Chemical Society 2019 141 (13), 5154-5158. doi: 10.1021/jacs.9b01561
PLOS ONE, 14(2), e0212011. doi: 10.1371/journal.pone.0212011
Chemical Reviews 2019 119 (1), 478-598. doi: 10.1021/acs.chemrev.8b00311
Transactions of the American Fisheries Society. doi:10.1002/tafs.10126
Proceedings of the National Academy of Sciences, 201807437. doi: 10.1073/pnas.1807437115.
Canadian Journal of Fisheries and Aquatic Sciences, 76(5), 762–779. doi: 10.1139/cjfas-2018-0008
Ocean & Coastal Management, 163, 240–253. doi:10.1016/j.ocecoaman.2018.06.016
Renewable and Sustainable Energy Reviews, 90, 945–956. doi: 10.1016/j.rser.2018.04.014
Marine and Coastal Fisheries, 10(2), 236–254. doi: 10.1002/mcf2.10021
Transactions of the American Fisheries Society, 147(3), 525–540. doi: 10.1002/tafs.10053
Energy, Sustainability and Society, 8(1). doi: 10.1186/s13705-018-0152-5
Nature Sustainability, 1(4), 184–189. doi: 10.1038/s41893-018-0050-z
Carsey Research National Fact Sheet, Carsey School of Public Policy, University of New Hampshire. National Fact Sheet No. 37
Nature Geoscience. doi: 10.1038/s41561-018-0069-9
Springer International Publishing. doi: 10.1007/978-3-319-65711-0.
Ocean and Coastal Management, 151: 53-60. doi: 10.1016/j.ocecoaman.2017.10.025
Agricultural and Forest Meteorology. doi: 10.1016/j.agrformet.2017.11.030
Ecology and Society, 22(4):19. doi: 10.5751/es-09733-220419
Ecology and Society 22(4):17. doi: 10.5751/es-09519-220417
Ecology and Society, 22(4). doi: 10.5751/es-09662-220418
Maine Policy Review, 26.2: 9-18.
Journal of Glaciology, 63(241): 877-887. doi: 10.1017/jog.2017.54
Water Alternatives, 10(3): 724-743.
Oxford Research Encyclopedia of Climate Science. doi: 10.1093/acrefore/9780190228620.013.442.
Resilience 2017 Conference Proceedings. Stockholm Waterfront Congress Centre, Sweden, August 20-23, 2017.
Resilience 2017 Conference Proceedings. Stockholm Waterfront Congress Centre, Sweden, August 20-23, 2017.
Geosciences, 7(3), 54. doi: 10.3390/geosciences7030054
Conference proceedings from the Association of Environmental Engineers and Science Professors (AEESP) Research and Education Conference, University of Michigan, Ann Arbor, Michigan, June 21-22, 2017.
Carsey Research Policy Brief, Carsey School of Public Policy, University of New Hampshire. National Issue Brief No. 123
Ecology and Society, 22(2), 39. doi: 10.5751/es-09105-220239. Part of a special feature on Ecosystems and Society: Interactions Among Climate, Land Use, Ecosystem Services, and Society.
Oxford Research Encyclopedia of Climate Science. doi: 10.1093/acrefore/9780190228620.013.563.
River Research and Applications, 33(7), 1004–1015. doi: 10.1002/rra.3155.
Society and Natural Resources, 1–16. doi:10.1080/08941920.2017.1315653
Environmental Communication: A Journal of Nature and Culture, 1-6. doi: 10.1080/17524032.2017.1308408
Biological Conservation, 208, 55-64. doi:10.1016/j.biocon.2016.07.019
Carsey Research National Fact Sheet, Carsey School of Public Policy, University of New Hampshire. National Fact Sheet No. 35.
Philosophy and Rhetoric 50(1), 1-25. doi: 10.5325/philrhet.50.1.0001
Limnology and Oceanography: Methods. doi:10.1002/lom3.10157
Journal of Geophysical Research: Atmospheres, 122(1), 121–139. doi: 10.1002/2016jd025362
Hydrological Processes, 31(5), 1074–1085. doi:10.1002/hyp.11091
Journal of Geophysical Research: Biogeosciences, 121(12), 3072–3088. doi:10.1002/2016jg003450
Ecosystem Services, 22, 213–220. doi:10.1016/j.ecoser.2016.11.007
Journal of Clinical Microbiology, 55(2), 645–648. doi:10.1128/jcm.02162-16
Journal of Geophysical Research: Atmospheres. doi:10.1002/2016jd025351
SAGE Open, 6(4), 215824401667629. doi:10.1177/2158244016676296
Water, 8(11), 522. doi:10.3390/w8110522
Global Change Biology, 23(4), 1610-1625. doi:10.1111/gcb.13517
Technical report summarizing research findings.
Ocean & Coastal Management, 130, 196–204. doi:10.1016/j.ocecoaman.2016.06.005
Journal of Visualized Experiments, 116. doi:10.3791/54704
Sociology, 50(5), 913-933. doi: 10.1177/0038038516648547
Journal of Climate, 29, 5141-5156. doi: 10.1175/jcli-d-15-0286.1
Great Bay Matters, Spring/Summer 2015
Geophysical Research Letters, 42(16), 6688–6695. doi: 10.1002/2015gl064965
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Carsey Research Policy Brief, Carsey School of Public Policy, University of New Hampshire. Regional Issue Brief No. 45
Ecology and Society, 21(3), 32. doi: 10.5751/ES-08680-210332
New Hampshire EPSCoR. 2.
Land, 5(3), 30. doi:10.3390/land5030030
Global Biogeochemical Cycles, 30(8), 1183-1191. doi: 10.1002/2016GB005468
Environmental Modelling and Software, 82, 7–20. doi: 10.1016/j.envsoft.2016.04.011
Ecosystem Services, 20, 104-112. doi: 10.1016/j.ecoser.2016.06.007
Hydrological Processes, 30(24), 4617-4632. doi: 10.1002/hyp.10956
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Carsey Research Policy Brief, Carsey School of Public Policy, University of New Hampshire. National Issue Brief No. 100
Ecology and Society, 21(2). doi: 10.5751/es-08437-210248
Applied Environmental Education & Communication, 15(3), 261–274. doi:10.1080/1533015x.2016.1181018
Carsey Research Policy Brief, Carsey School of Public Policy, University of New Hampshire. National Issue Brief No. 99
PLOS ONE, 11(5), e0155018. doi:10.1371/journal.pone.0155018
Journal of Physical Oceanography, 46(5), 1421–1436. doi: 10.1175/jpo-d-13-0271.1
Public Understanding of Science, 25(4), 415–426. doi:10.1177/0963662516629750
Conservation Biology, 30(6), 1173-1181. doi: 10.1111/cobi.12745
Cold Regions Science and Technology, 123, 149–154. doi: 10.1016/j.coldregions.2015.11.018
Elementa: Science of the Anthropocene, 4, 000090. doi: 10.12952/journal.elementa.000090
Frontiers Ecology and the Environment, 14(1), 46–52. doi: 10.1002/16-0113.1
Regional Environmental Change, 16(9), 1819-1832. doi: 10.1007/s10113-015-0914-y
Journal of Hydraulic Engineering, 142(2), 06015019. doi:10.1061/(asce)hy.1943-7900.0001079
Ecological Applications, 26(1), 146-161. doi: 10.1890/14-2207
In Stream Ecosystems in a Changing Environment (pp. 349–388). Elsevier. doi: 10.1016/B978-0-12-405890-3.00008-7
Journal of Applied Communication Research, 44(1), 78–95. doi:10.1080/00909882.2015.1116707
Reflections: A Journal of Public Rhetoric, Civic Writing, and Service Learning, 16(1), 75-95
Technical report provided to the Campus Compact and Campuses for Environmental Stewardship program
Technical Report. Luc Hoffmann Institute, Pew Charitable Trusts, California Ocean Science Trust, Science and Resilience Institute at Jamaica
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