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Addis Ababa University
1.
Gebremedhn, Elias.
Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
.
Degree: 2012, Addis Ababa University
URL: http://etd.aau.edu.et/dspace/handle/123456789/712
► Abstract: The behavior of the ground and the first two excited states of the compound 4-(N,N-dimethylamino)-benzonitrile (4DMABN) have been studied using both experimental and theoretical…
(more)
▼ Abstract: The behavior of the ground and the first two excited states of
the compound 4-(N,N-dimethylamino)-benzonitrile (4DMABN) have been
studied using both experimental and theoretical methods. For
comparison purpose the ground and the first two excited states of the
compounds 3-(N,N-dimethyl amino)-benzonitrile (3DMABN) and 2,3,6,7-
tetrahydro-1H,5H-pyridol[3,2,1-ij]quinoline-9-carbonitrile (TMABN) have
been studied theoretically. The experimentally achieved absorption
spectrum of 4DMABN has shown two distinct bands. And the emission
spectrum has also two distinct bands, the behavior of which is
dependent on the wavelength of the exciting light. This is attributed to
the presence of two stable conformers of the compound in the ground
state. Excited state calculations using TDDFT method have shown that
the first two excited states of the compound 4DMABN have different
properties in the gaseous and the solvated system. This is in agreement
with the experimental result that the compound shows two emission
bands in the solvent acetonitrile and one band in the gaseous state. The
same theoretical calculation has shown higher excitation energy to the S2
state at the perpendicular conformation of the compound 3DMABN. This
agrees with the absence of a CT band in experiment. For the compound
TMABN the same calculation has shown for the existence of only one
emitting excited electronic state at a considerably twisted conformation.
This is in agreement with the experimentally found single CT band.
Advisors/Committee Members: Dr. Ahmed Mustefa (advisor).
Subjects/Keywords: Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Gebremedhn, E. (2012). Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
. (Thesis). Addis Ababa University. Retrieved from http://etd.aau.edu.et/dspace/handle/123456789/712
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Gebremedhn, Elias. “Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
.” 2012. Thesis, Addis Ababa University. Accessed January 16, 2021.
http://etd.aau.edu.et/dspace/handle/123456789/712.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Gebremedhn, Elias. “Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
.” 2012. Web. 16 Jan 2021.
Vancouver:
Gebremedhn E. Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
. [Internet] [Thesis]. Addis Ababa University; 2012. [cited 2021 Jan 16].
Available from: http://etd.aau.edu.et/dspace/handle/123456789/712.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Gebremedhn E. Computational and Experimental Study on the Dual Fluorescence Phenomenon of 4-(N, N-dimethylamino)- benzonitrile and Related Compounds
. [Thesis]. Addis Ababa University; 2012. Available from: http://etd.aau.edu.et/dspace/handle/123456789/712
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Stellenbosch University
2.
Geswindt, Theodor Earl.
Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium.
Degree: PhD, Chemistry and Polymer Science, 2013, Stellenbosch University
URL: http://hdl.handle.net/10019.1/85647
► ENGLISH ABSTRACT: In this thesis, the recovery of RhIII from both synthetically prepared and authentic industrial PGM-containing solutions was systematically investigated via organic precipitation methods…
(more)
▼ ENGLISH ABSTRACT: In this thesis, the recovery of RhIII from both synthetically prepared and authentic
industrial PGM-containing solutions was systematically investigated via organic precipitation
methods using several commercially available, N-containing organic receptors including
(amongst others) diethylenetriamine (Deta), triethylenetetramine (Teta),
tetraethylenepentamine (Tepa) and tris(2-aminoethyl)amine (Tren). These organic receptors
act as precipitating agents in the presence of an appropriate protonating agent (HCl) by
lowering the solubility of the PGM chlorido-anions through an ion-pairing mechanism. The
recovery of RhIII from synthetically prepared PGM (RhIII and PtIV) containing solutions using
these precipitants was excellent, while poor Rh recovery from authentic industrial process
solutions was achieved. The poor Rh recovery from these process solutions was ascribed to
the species distribution of the [RhCln(H2O)6-n]3-n complexes. In order to validate the
proposition that RhIII speciation effects are responsible for the poor Rh recovery observed
during the precipitation studies, attempt were made to describe the species distribution of the
[RhCln(H2O)6-n]3-n (n=3-6) by means of high-resolution 103Rh NMR spectroscopy.
A detailed high-resolution 103Rh NMR spectroscopic study of the series of
[RhCln(H2O)6-n]3-n (n=3-6) complexes was conducted. During this study, all six RhIII aqua
chlorido-complexes have unambiguously been characterized by means of high-resolution
103Rh NMR spectroscopy, proving the powerful analytical capability of this technique.
Characterization of these complexes is based on the detailed analysis of the 35Cl/37Cl isotope
effects which is observed in the 19.11 MHz 103Rh NMR resonances of the [RhCln(H2O)6-n]3-n
(n=3-6) complexes in aqueous HCl solutions at 292 K. These resonances show that the “finestructure”
of each of the 103Rh resonances may be understood in terms of its unique
isotopologue, and in certain cases, the isotopomer distribution of each complex, which
manifests as a result of its statistically expected 35Cl/37Cl isotopologue and isotopomer
distributions. As a result, the 103Rh NMR resonance structure serves as a unique “NMRfingerprint”,
which allows for the unambiguous assignment of [RhCln(H2O)6-n]3-n (n=3-6)
complexes, without the reliance on accurate δ(103Rh) chemical shifts.
Furthermore, this study reports the first direct species distribution diagram for the
[RhCln(H2O)6-n]3-n (n=3-6) series of complexes (in aqueous HCl solutions at 292 K) as a function of the “free” (unbound) chloride concentration, constructed from 103Rh NMR
measurements. The need for a revised speciation diagram of [RhCln(H2O)6-n]3-n (n=3-6)
complexes is clearly reflected by the vast differences observed in the literature reported
species distribution diagrams, which makes it difficult to decide which set of experimental
conditions (if any) is required for the quantitative and “selective” recovery of RhIII from
aqueous HCl solutions containing associated PGMs (Pt,…
Advisors/Committee Members: Koch, Klaus R., Stellenbosch University. Faculty of Science. Dept. of Chemistry and Polymer Science..
Subjects/Keywords: Chemistry; Department of Chemistry and Polymer Science
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Geswindt, T. E. (2013). Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium. (Doctoral Dissertation). Stellenbosch University. Retrieved from http://hdl.handle.net/10019.1/85647
Chicago Manual of Style (16th Edition):
Geswindt, Theodor Earl. “Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium.” 2013. Doctoral Dissertation, Stellenbosch University. Accessed January 16, 2021.
http://hdl.handle.net/10019.1/85647.
MLA Handbook (7th Edition):
Geswindt, Theodor Earl. “Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium.” 2013. Web. 16 Jan 2021.
Vancouver:
Geswindt TE. Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium. [Internet] [Doctoral dissertation]. Stellenbosch University; 2013. [cited 2021 Jan 16].
Available from: http://hdl.handle.net/10019.1/85647.
Council of Science Editors:
Geswindt TE. Chemical speciation of RhIII complexes in acidic, halide-rich media by means of 103Rh NMR spectroscopy : the importance of speciation in the selective separation and recovery of rhodium. [Doctoral Dissertation]. Stellenbosch University; 2013. Available from: http://hdl.handle.net/10019.1/85647

University of Zurich
3.
Gatti, Michele.
New catalysts and new substrates in ring-closing metathesis.
Degree: 2011, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/57171/1/20111264.pdf
► In den letzten 20 Jahren entwickelte sich die Olefin-Metathese zu einer ausgezeichneten Methode um Kohlenstoff-Kohlenstoff Doppelbindungen zu manipulieren. Trotz des ernormen Fortschritts bezüglich Stabilität von…
(more)
▼ In den letzten 20 Jahren entwickelte sich die Olefin-Metathese zu einer ausgezeichneten Methode um Kohlenstoff-Kohlenstoff Doppelbindungen zu manipulieren. Trotz des ernormen Fortschritts bezüglich Stabilität von Katalysatoren, deren hohe Aktivitäten und deren Toleranz gegenüber funktionellen Gruppen sind weitere Verbesserungen von grosser Bedeutung. Diese Dissertation ist dem Ziel gewidmet neuartige Katalysatoren zu synthetisieren und deren Verhalten in der Ringschlussmethatese (RCM) zu untersuchen. Der erste Abschnitt dieser Arbeit, welcher im zweiten Kapitel beschrieben ist, konzentriert sich auf die Entwicklung von einer Reihe auf Ruthenium basierende Metathesekatalysatoren der Hoveyda-Blechert-Familie. Diese Katalysatoren bestehen aus N-heterozyklische Carbene mit einer substituierten Naphthyl-Seitenkette. Zum ersten Mal war eine chromatographische Trennung und Aufreinigung der syn- und anti-Isomere einiger Katalysatoren erfolgreich. Durch verschiedene kinetische Untersuchungsreihen an den isolierten Isomeren konnten entscheidende Unterschiede in der Aktivität und Stabilität zwischen anti- und syn-Konformeren des Katalysators festgestellt werden. Intensive Studien zur Auswirkung der Konzentration auf die Reaktionsrate von RCM-Reaktionen wurden zusätzlich durchgeführt mit dem Ergebnis, dass unter bestimmten Konditionen, sehr hohe Konzentrationen des Vorläufer-Diens zu RCM führen kann mit einer Vielfalt von Substraten mit extrem niedrig katalytischer Ladung. Im dritten Kapitel wird die Synthese und Charakterisierung einer neuen Familie von NHC mit mono- oder disubstituierten Seitenketten behandelt. Das Ziel dieser Arbeit war das Erlangen von Liganden, welche vorwiegend die anti–Konformation einnehmen. Dadurch wird erreicht, dass diese Komponenten vielseitiger in der Organischen Chemie und als Organokatalysatoren einsetzbar sind. Insbesonders können durch Inkorporation der Liganden diese Ru-Katalysatoren zu Metathese-Reaktionen verwendet werden. Im vierten Kapitel wird zum Abschluss die Entwicklung jener katalytischen Methoden, um Alkenbromide durch RCM-Reaktionen zu erhalten, angestrebt. Dafür werden katalytische Mengen von kommerziell erwerblichen Katalysatoren verwendet. Diese Produkte stellen ein grosses Interesse, nicht nur als Bausteine in der Organischen Synthese dar, sondern auch als Möglichkeit neuwertige milde synthetische Wege einzuschlagen. Eingeschlagene Versuche diese Reaktionsmechanismen zu klären werden in dieser Arbeit vorgestellt.
In the past twenty years, olefin metathesis has developed into an excellent method to manipulate carbon-carbon double bonds. Despite the enormous progress in terms of stability of catalysts, their activities and their high tolerance of functional groups, further improvements are of great importance. The aim of this dissertation is to synthesize novel catalysts and investigate their behavior in ring closing metathesis reactions (RCM). The first section of this work, which is described in the second chapter, focuses on the development of a series of…
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Gatti, M. (2011). New catalysts and new substrates in ring-closing metathesis. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/57171/1/20111264.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Gatti, Michele. “New catalysts and new substrates in ring-closing metathesis.” 2011. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/57171/1/20111264.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Gatti, Michele. “New catalysts and new substrates in ring-closing metathesis.” 2011. Web. 16 Jan 2021.
Vancouver:
Gatti M. New catalysts and new substrates in ring-closing metathesis. [Internet] [Thesis]. University of Zurich; 2011. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/57171/1/20111264.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Gatti M. New catalysts and new substrates in ring-closing metathesis. [Thesis]. University of Zurich; 2011. Available from: https://www.zora.uzh.ch/id/eprint/57171/1/20111264.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
4.
Romanato, Paola.
Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination.
Degree: 2011, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/57172/1/20111270.pdf
► Silyliumionen sind höhere Analoge von Carbokationen der Struktur R3Si+. Was sie vor allem auszeichnet, ist ihre enorme Elektrophilie. Die Erzeugung langlebiger silylkationen hat deshalb die…
(more)
▼ Silyliumionen sind höhere Analoge von Carbokationen der Struktur R3Si+. Was sie vor allem auszeichnet, ist ihre enorme Elektrophilie. Die Erzeugung langlebiger silylkationen hat deshalb die Entwicklung neuartiger synthetischer Wege und schwach nucleophile Reaktionsbedingungen bedingt. Erst 2002 wurden mit der Kristallstruktur eines Triarylsilyliumions letzte Zweifel an der Existenz dreifach koordinierter Siliziumkationen ausgeräumt. In den vergangenen Jahren haben verschiedene Forschungsgruppen Silyliumionen erfolgreich zur Erzeugung reaktiver Zwischenstufen und in der Lewissäure-Katalyse angewandt.
Das Ziel dieser Arbeit ist die Erweiterung der Familie dieser Terphenylsilyiumionen, die in der Siegel Gruppe bereits entwickelt wurden. Die Terphenylgrundstruktur bietet sterische Abschirmung von der positiven Ladun des Siliciumkerns sowie eine komplette thermodynamsiche Stabilisierung durch die pie-Koordination. Um die Lewis-Acidität zu regeln, wurde die Elektronendichte der benachbarten Ringe reduziert. Zuerst wurden Halogenatome an der ortho-Position dieser benachbarten Ringe eingeführt Diese mindern die Koordination der pie-Arene, so dass eine bevorzugte Koordination zwischen dem Halogen und dem Silicium stattfinden. Diese Konformation wurde durch NMR, X-Ray und Berechnungsmethoden bestätigt.
Eine zweite Generation von Terphenylsilyliumionen wurde synthetisiert, mit Halogenatome in para-Position zu der benachbarten Ringen. Somit sollte eine Koordination am lateralen Ring und an den Halogenatomen vermieden werden wodurch das Silyiumion entschirmt wird. Durch Verwendung von X-Ray- Kristallographie wurde gezeigt, dass die intramolekulare Koordination des positiv geladenen Kerns mit den benachbarten Ringen tatsächlich reduziert wurde und dass die intermolekulare Koordination mit dem Gegenion konkurriert.
Durch ein grosses Interesse die Energetik der pie-Arene-Koordinationen detailliert zu erforschen, wurden eine Reihe von Kationen aus 2,6-Difluoro- und 2,6-Dimethyl-substitutierte Ringe synthetisiert. Somit wurde die Koordination zwischen den abgeschiedenen Halogenpaar zu Silicium verglichen. Dabei wurde bedeutsamerweise eine Konkurrenz anstatt einer Kooperation zwischen den beiden Stabilisierungsmethoden erkannt. Eine Interaktion von F=>Si wird durch methylierte Ringe mit niedrigere Basizität, wohingegen eine pie-Koordination mit duryl- und pentamethylphenyl-Substituenten bevorzugt wird.
In dieser Arbeit wurde erfolgreich eine neue Art der Phenylsilyiumionen, die sterisch zugänglichere trikoordinierte Triarylsilyliumionen widerspiegeln, synthetisiert und untersucht. Diese Strukturen weisen niedrige Resonanzverschiebung in 29Si- NMR Spektroskopie auf, was ein klares Zeichen von abgeschirmten kationischen Zentren darstellt. Die Stabilität dieser „nackten“ Silyliumionen ist auf die agostische Wechselwirkung mit den benachbarten aliphatischen Gruppen zurückzuführen. Eine erst kürzlich aufgesetzte Hypothese befasst sich mit Kationen, die in eine stabilere Triarylsilylkation-Struktur neu geordnet werden. Diese sind…
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Romanato, P. (2011). Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/57172/1/20111270.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Romanato, Paola. “Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination.” 2011. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/57172/1/20111270.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Romanato, Paola. “Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination.” 2011. Web. 16 Jan 2021.
Vancouver:
Romanato P. Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination. [Internet] [Thesis]. University of Zurich; 2011. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/57172/1/20111270.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Romanato P. Intramolecular stabilization of 2,6-diarylphenylsilylium ions by π-arene and lone pair-halogen coordination. [Thesis]. University of Zurich; 2011. Available from: https://www.zora.uzh.ch/id/eprint/57172/1/20111270.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
5.
Seyfried, M S.
Design and synthesis of planar telomestatin analogs.
Degree: 2011, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/58123/1/Dissertation_Seyfried.pdf
► Telomestatin is a natural product isolated from Streptomyces anulatus 3533-SV4. It is one of the most potent telomerase inhibitors reported to date, and it exhibits…
(more)
▼ Telomestatin is a natural product isolated from Streptomyces anulatus 3533-SV4. It is one of the most potent telomerase inhibitors reported to date, and it exhibits a broad range of biological activities.
The proposed mode of action of telomestatin involves selective binding of G-quadruplex structures present in the 3' telomeric overhang of human chromosomes. The high affinity and specificity of telomestatin for G-quadruplex DNA is rationalized by its size and shape complementarity with the G-tetrads of G-qadruplex DNA. In reality, the shape of telomestatin is not perfect for G-tetrad stacking due to the presence of a single thiazoline unit. This makes telomestatin a non-planar molecule. Due to high macrocyclic ring-strain, all attempts to synthesise a macrocycle containing eight azole-units have thus far proven fruitless. Ring-stain is reduced by replacing four oxazole units with thiazole in the macrocyclic system. We therefore pursued the synthesis of three new, fully planar telomestatin analogs, each containing four thiazoles and the remaining units comprising oxazoles, imidazoles or thiazoles. The following work presents the design and the synthetic efforts towards these target molecules starting with three different amino acids: serine, asparagine and cysteine.
Our synthetic strategy involves the coupling of amino acids followed by cyclodehydration reactions. The resulting azole-containing amino acids are tetramerized and macrolactamized using standard peptide chemistry. The remaining amino acid side chains are then used for four cyclodehydration reactions in a single step. In 18 synthetic steps total, the C4-symmetric 4TOP could be synthesised. This is the first macrocyclic compound containing eight azole units ever reported. Along the way towards this challenging goal, new synthetic methodologies were developed including the use of silyl-protected alcohols for cyclodehydration reactions, as well as a highly efficient and mild method for 18O labelling of protected amino acids.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Seyfried, M. S. (2011). Design and synthesis of planar telomestatin analogs. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/58123/1/Dissertation_Seyfried.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Seyfried, M S. “Design and synthesis of planar telomestatin analogs.” 2011. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/58123/1/Dissertation_Seyfried.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Seyfried, M S. “Design and synthesis of planar telomestatin analogs.” 2011. Web. 16 Jan 2021.
Vancouver:
Seyfried MS. Design and synthesis of planar telomestatin analogs. [Internet] [Thesis]. University of Zurich; 2011. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/58123/1/Dissertation_Seyfried.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Seyfried MS. Design and synthesis of planar telomestatin analogs. [Thesis]. University of Zurich; 2011. Available from: https://www.zora.uzh.ch/id/eprint/58123/1/Dissertation_Seyfried.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
6.
Huber, S M.
Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity.
Degree: 2012, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/71542/1/Master_Thesis_Sabrina_Huber_May_2012.pdf
► DNA quadruplex structures are attracting great scientific interest because of increasing evidence that these structures play important roles in biological processes ranging from replication, transcription,…
(more)
▼ DNA quadruplex structures are attracting great scientific interest because of increasing evidence that these structures play important roles in biological processes ranging from replication, transcription, and recombination to telomere integrity. The use of small molecules to selectively target these structures in vivo is emerging as a promising way to interfere with telomere replication in tumor cells and provides potential anticancer agents. A large number of quadruplex binding ligands have already been reported. In general, they selectively interact with terminal GGGG-tetrads via π-π stacking interactions. However, in addition to GGGG-tetrads, GCGC-tetrads are known to be involved in quadruplex formation in vitro. Even though these so-called “mixed tetrads” might also have biological relevance, selective GCGC-tetrad binding probes have not yet been reported.
Hemiporphyrazines (Hps) are non-aromatic, 20 π-electron phthalocyanine (Pc) derivatives that consist of two co-facial pyridine rings and two co-facial isoindole units linked through four aza bridges. Due to their planarity, extended π-conjugation, and C2-type symmetry, they are good candidates for selectively targeting GCGC-tetrads. Unsubstituted Hps are, however, notoriously insoluble materials and therefore little is known about their chemical and photophysical properties. As a consequence, this Master thesis is focused on the synthesis, structure, photophysical and reactivity properties of Hps to assess their potential as future GCGC-tetrad binding ligands.
Free-base hemiporphyrazine (HpH2) was synthesized and its structure was analyzed by single crystal X-ray diffraction. HpH2 adopts a nearly planar structure and its macrocyclic core contains alternating double and single bonds. This is consistent with the non-aromatic character of these compounds. Furthermore, HpH2 has a very high water affinity and readily absorbs water from the atmosphere to form a yellow monohydrate (HpH2·H2O). This compound has a saddle-shaped conformation and distinct photophysical properties. The use of bulky metal triflates (M(OTf)2) as sources of metal ions during macrocyclization furnished metallo Hps (MHps) with enhanced solubility properties. Octahedral zinc and nickel trans-ditriflate hemiporphyrazine complexes “HpH2Zn(OTf)2” and “HpH2Ni(OTf)2” provide two such examples.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Huber, S. M. (2012). Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/71542/1/Master_Thesis_Sabrina_Huber_May_2012.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Huber, S M. “Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity.” 2012. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/71542/1/Master_Thesis_Sabrina_Huber_May_2012.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Huber, S M. “Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity.” 2012. Web. 16 Jan 2021.
Vancouver:
Huber SM. Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity. [Internet] [Thesis]. University of Zurich; 2012. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/71542/1/Master_Thesis_Sabrina_Huber_May_2012.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Huber SM. Hemiporphyrazines: Synthesis, Photophysical Properties and Reactivity. [Thesis]. University of Zurich; 2012. Available from: https://www.zora.uzh.ch/id/eprint/71542/1/Master_Thesis_Sabrina_Huber_May_2012.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
7.
Can, Daniel.
An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core.
Degree: 2012, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/74763/1/20131778.pdf
► The chemical and biological evaluation of organometallic probes for nuclear medical applications in comparison to their purely organic analogs, or the study of the metal-mediated…
(more)
▼ The chemical and biological evaluation of organometallic probes for nuclear medical applications in comparison to their purely organic analogs, or the study of the metal-mediated retro-Diels-Alder behaviour of derivatized cyclopentadienyl dimers is an overarching description of this thesis. Focussing on the synthesis of 99mTc- labelled radiopharmaceuticals and the corresponding cold rhenium-compounds, a variety of organic and inorganic cyclopentadienyl derivatives have been synthesized. Arylsulfonamides, -sulfamides and -sulfamates for the targeting of human carbonic anhydrase IX, hydroxamic acids acting as HDAC-inhibitors, organometallic antibiotics or catechol amine derivatives have been studied. Organometallic complexes with bioactive ligands are nowadays interesting for both, the noninvasive imaging of biological features and the therapeutic treatment of diseases. While several transition metals across the periodic table are frequently used for therapy, 99mTc is the most prominent nuclide in nuclear medical diagnostics. It would be desirable, in a theragnostics sense (therapy and diagnostics), to have identical compounds for combined therapy and non-invasive diagnosis. Among transition-metals, rhenium and technetium belong to the same triad. Therefore it is possible to use identical compounds for combined therapy and imaging. While Re- based compounds can be used for therapy, the homologous compounds with 99mTc can serve as imaging agents for Single Photon Emission Computed Tomography (SPECT). [(CpR)M(CO)3]-type compounds are considered as very stable complexes under various conditions and can synthetically be treated like aromatic organic molecules. Re-compounds are therefore usually synthesized starting from [(Cp)Re(CO)3] and using standard organic synthesis procedures, whereas for the corresponding 99mTc- complexes, the uncoordinated HCp-ligand is prepared prior to complexation, either as a monomer or in its dimeric form.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Can, D. (2012). An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/74763/1/20131778.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Can, Daniel. “An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core.” 2012. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/74763/1/20131778.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Can, Daniel. “An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core.” 2012. Web. 16 Jan 2021.
Vancouver:
Can D. An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core. [Internet] [Thesis]. University of Zurich; 2012. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/74763/1/20131778.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Can D. An Approach Towards Theragnostic Receptor Targeting with 5-Cyclopentadienyl Derivatives of the fac-{99mTc(CO)3}- and fac-{Re(CO)3}-Core. [Thesis]. University of Zurich; 2012. Available from: https://www.zora.uzh.ch/id/eprint/74763/1/20131778.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
8.
Barman, Samir.
Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing.
Degree: 2012, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/75114/1/20131675.pdf
► Poröse metallorganische Gerüste (engl. metal-organic frameworks, MOFs) wurden in den letzten Dekaden, auf Grund ihrer hohen spezifischen Oberfläche, abstimmbarer Porengrösse, funktionalisierbarer Porenwände und definierter Wasserstoffbindungstellen,…
(more)
▼ Poröse metallorganische Gerüste (engl. metal-organic frameworks, MOFs) wurden in den letzten Dekaden, auf Grund ihrer hohen spezifischen Oberfläche, abstimmbarer Porengrösse, funktionalisierbarer Porenwände und definierter Wasserstoffbindungstellen, intensiv als vielversprechendes Wasserstoffspeichermaterial untersucht. Neuere Ergebnisse belegen, dass MOFs mit grosser Oberfläche und hoher Porosität bis zu 10-15 Gew.-% Wasserstoff bei Flüssig- Stickstoff-Temperatur und 40-80 bar Wasserstoffdruck liefern können. Die Speicherkapazität bei Raumtemperatur, die wahrscheinlich bedeutend für praktische Anwendung wäre, sinkt dazu im Gegensatz dramatisch unter ein Zehntel der Kapazität bei tiefem Temperaturen. Der Hauptgrund hierfür ist, dass die Wasserstoffadsorption in MOFs durch Physisorptionsprozesse geschieht und daher nur schwache van-der-Waals-Kräfte die primäre Bindungskraft bilden. Verschiedene Ansätze haben kürzlich gezeigt wie Bindungskräfte zwischen MOFs und Wasserstoff verstärkt werden können, um so signifikante Mengen Wasserstoff bei relativ höheren Temperaturen zu liefern. Basierend auf neueren bekannten Ergebnissen, entwickelten wir chemisch abstimmbare, poröse MOFs durch rationelles Design der organischen Bausteine der Materialien oder durch Anbringung geeigneter chemischer Bausteine an die Oberflächer der funktionelle Gruppen tragenden MOFs. Die chemische Abstimmung scheint bedeutend, um fortgeschrittene polare Bindungen durch Dipol-Dipol- oder Dipol-induzierter Dipol-Wechselwirkungen oder Wasserstoffbindungen in Verbindung mit kinetischem Einfangen der Wasserstoffmoleküle zu sein. Im Besonderen hat die hier präsentierte Forschungsarbeit das systematische Design, Synthese und postsynthetische Modifikation von MOFs für Wasserstoffspeicherung und den sensitiven Nachweis von nitroaromatischen Sprengstoffen untersucht. Um den Effekt der Polarisierung auf die Stabilisierung von Wasserstoff in MOFs zu untersuchen, wurde eine Reihe neuer MOFs, basierend auf polarisierten Azulenliganden, entwickelt und ihre Wasserstoffspeichereigenschaften wurden intensiv untersucht. Zusätzlich konnte eine neue Methode für die postsynthetische Modifikation amin-funktionalisierter MOFs zur Einführung polarisierter Gruppen durch Gasphasen-Festphasen-Reaktionen aufgezeigt werden. Des Weiteren wurde eine innovative Strategie zu Einführung hoher Konzentrationen von vakanten Metallbindungstellen untersucht. Die Anwesenheit die Metallbindungsstellen wurde als förderlich für die Unterstützung von Wasserstoffmolekülen nachgewiesen. In einer weiteren Studie haben wir 3D-formbeständige organische Rezeptoren basierend auf Triptycentetracarboxylat für den hochselektiven und hochsensitiven Nachweis von Sprengstoffen duch lichtinduzierten Elektronentransfer-Quenching-Mechanismus angewendet. Zusammenfassend betrachtet, hat diese Doktorarbeit zum Feld der Wasserstoffspeicherung und der Nutzung von MOFs als Chemosensoren beigetragen.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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Record Details
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Barman, S. (2012). Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/75114/1/20131675.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Barman, Samir. “Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing.” 2012. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/75114/1/20131675.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Barman, Samir. “Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing.” 2012. Web. 16 Jan 2021.
Vancouver:
Barman S. Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing. [Internet] [Thesis]. University of Zurich; 2012. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/75114/1/20131675.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Barman S. Design, synthesis and postsynthetic modification of metal-organic materials for hydrogenstorage and chemosensing. [Thesis]. University of Zurich; 2012. Available from: https://www.zora.uzh.ch/id/eprint/75114/1/20131675.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
9.
Shen, Yunjun.
Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging.
Degree: 2014, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/90842/1/20142053.pdf
► Im Rahmen dieser Arbeit wurde eine Reihe von kleinen, tripodalen Liganden mit verschiedenen funktionellen Gruppen konzipiert und synthetisiert. Die resultierenden Komplexe mit der [99mTc(CO)3]+ Einheit…
(more)
▼ Im Rahmen dieser Arbeit wurde eine Reihe von kleinen, tripodalen Liganden mit verschiedenen funktionellen Gruppen konzipiert und synthetisiert. Die resultierenden Komplexe mit der [99mTc(CO)3]+ Einheit sind klein und hydrophil. Des Weiteren wurden diverse Glucose Derivate synthetisiert, welche an den Positionen C1, C2, C3 und C6 über einen PEG Linker mit dem 1,2-Diaminopropionsäure Chelator 99m funktionalisiert sind. Markierungs-Studien mit Tc waren selbst bei tiefen Glucose Konzentrationen möglich. Die Zellaufnahme von den entsprechenden 99mTc Komplexen wurde in verschiedenen Tumorzelllinien untersucht. Dabei wurde eine schlechte bis moderate Zellaufnahme für die verschiedenen Glucose Derivate beobachtet. Aufgrund der Tatsachte, dass keine signifikante Hemmung der Zellaufnahme in der Gegenwart von Cytochalasin B oder 2-Deoxy-D-Glucose gefunden wurde, ist eine unspezifische Zellaufnahme offensichtlich und nicht ein aktiver Transport in die Zelle über den GLUT-1 Transporter. Um die Chelatoren in Peptidsequenzen einzufügen, wurde die Aminogruppe an der ε- Position von L-Lysine durch die tripodalen Liganden ersetzt oder die Carbonsäure γ- Position von Glutaminsäure über einen PEG Linker mit dem tripodalen Liganden verbunden. Die sogenannten orthogonal geschützten „Single Amino Acid Chelates (SAACs)“ wurden entweder an den N- und C-Terminus von Bombesin angehängt oder direkt in die Sequenz integriert mittels Festphasenpeptidsynthese. Ausserdem wurden die Aminosäurederivate in ein zyklisches RGD Peptid inkorporiert. Die verschiedenen Peptide konnten bei μM-Konzentrationen quantitativ mit der [99mTc(CO)3]+ Einheit markiert werden. Die Bestimmung der Affinität zum αvβ3-Integrin Rezeptor zeigte geringe bis mittelmässige Werte im nM Bereich für diverse Rezeptor-Subtypen. Die Biodistributionsstudien in Nacktmäusen mit einem M21 Melanom ergab eine vernünftige αvβ3-Integrin spezifische Tumoraufnahme.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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Record Details
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Shen, Y. (2014). Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/90842/1/20142053.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Shen, Yunjun. “Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging.” 2014. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/90842/1/20142053.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Shen, Yunjun. “Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging.” 2014. Web. 16 Jan 2021.
Vancouver:
Shen Y. Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging. [Internet] [Thesis]. University of Zurich; 2014. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/90842/1/20142053.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Shen Y. Synthesis of metal-containing biomolecule conjugates for potential use in 99mTc molecular imaging. [Thesis]. University of Zurich; 2014. Available from: https://www.zora.uzh.ch/id/eprint/90842/1/20142053.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
10.
Schnabl, Joachim Anton.
Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates.
Degree: 2013, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/91034/1/20152366.pdf
► Teil I Supramolekulare zweikernige Eisen(II)-Komplexe [Fe 2 L3 ]4+ sind helikale Zylinder die dank ihren ausserordentlichen DNS Bindungseigenschaften potentielle Antikrebsmittel sind. Die Zylinder können einerseits…
(more)
▼ Teil I Supramolekulare zweikernige Eisen(II)-Komplexe [Fe 2 L3 ]4+ sind helikale Zylinder die dank ihren ausserordentlichen DNS Bindungseigenschaften potentielle Antikrebsmittel sind. Die Zylinder können einerseits spezifisch an Y-förmige dreiarmige DNS Kreuzungen binden. Es wurde aber auch eine Anlagerung an die grosse Furche doppelsträngiger DNS gezeigt. Die geeignete Grösse und Form der Helikate sowie ihre hohe elektrostatische Ladung sind verantwortlich für diese nichtkovalenten Wechselwirkungen. Behandlung von Krebszelllinien mit den zylinderförmigen Komplexen resultierten in erhöhten Zellsterblichkeitsraten ohne das Erbgut der Zellen zu schädigen. Dieser alternative Mechanismus des Eisen(II) Supramoleküls könnte ein vielversprechender Schritt in Richtung Behandlung von Krebs sein, welcher schon Resitenzen gegen andere Chemotherapeutika aufweist. Die nichtkovalente Art der Erkennung von dreiarmigen Kreuzungen könnte somit die Entwicklung neuartiger Medikamente ermöglichen. RNS erfüllt verschiedene regulatorische Funktionen in einer Zelle. Da DNS und RNS eine sehr ähnliche Struktur aufweisen, stellte sich die Frage ob der Zylinder auch an RNS binden würde. RNS kommt meist als einzelsträngiges Molekül vor welches ein hohes natürliches Vorkommen an dreiarmigen Kreuzungen als potentielle Zielbindungsstellen enthält Die Beeinflussung der RNS in lebenden Zellen könnte ein Schlüsselelement in der Antitumoraktivität des Zylinders sein. In der ersten Studie dieser Dissertation wurden deshalb verschiedene RNS Konstrukte künstlichem oder natürlichem Ursprungs als Ziel für die Eisen(II) Zylinder verwendet. Das RNS Analogon der kürzlich entdeckten dreiarmigen DNS Kreuzung konnten erfolgreich kristallisiert und die Struktur mittels Röntgenkristallografie charakterisiert werden. Ferner wurden zwei weitere Kristallstrukturen der dreiarmigen RNS Kreuzung mit Kobalt(II) und Nickel(II) Zylindern gelöst. Diese drei Kristallstrukturen haben eine identische Topologie. Der Metallzylinder befindet sich im Zentrum der dreiarmigen RNS Kreuzung. Die inneren Ringe der aromatischen Liganden des Zylinders sind in π-Stapelwechselwirkung mit den zentralen Basenpaaren der RNS, die als drei Doppelhelices vom Inneren der dreiarmigen Kreuzung wegführt. Ein Vergleich der bekannten Kristallstruktur der dreiarmige DNS Kreuzung mit der dreiarmige RNS Kreuzung zeigt einen strukturellen Unteschied: Die enge Öffnung an der einen Seite der dreiarmigen DNS Kreuzung beschränkt die innere Platzierung des Zylinders auf eine gewisse Tiefe. Der Zylinder kann aber mit der dreiarmigen RNS Kreuzung eine maximale π-Stapeloberfläche einnehmen: beide Öffnungen der Kreuzung sind weit genug für eine freie Beweglichkeit des Zylinders und ermöglichen somit eine energetisch optimale Geometrie. Dies ist die erste Charakterisierung einer induzierten dreiarmigen RNS Kreuzung, die spezifisch durch einen supramolekularen Zylinder erkannt wurde. Teil II Tertiärstrukturen grosser Polyanionen wie DNS oder gerade RNS (z.B. Ribozyme) schliessen eine hochkomplexe dreidimensionale…
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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Record Details
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Schnabl, J. A. (2013). Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/91034/1/20152366.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Schnabl, Joachim Anton. “Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates.” 2013. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/91034/1/20152366.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Schnabl, Joachim Anton. “Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates.” 2013. Web. 16 Jan 2021.
Vancouver:
Schnabl JA. Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates. [Internet] [Thesis]. University of Zurich; 2013. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/91034/1/20152366.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Schnabl JA. Studies on the stabilization of RNA structures through metal ions, ion-π interactions and metallo-supramolecular helicates. [Thesis]. University of Zurich; 2013. Available from: https://www.zora.uzh.ch/id/eprint/91034/1/20152366.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
11.
Capolicchio, Samanta.
Synthesis of Diphosphoinositol Polyphosphates.
Degree: 2015, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/106364/1/20152470.pdf
► Diphosphoinositol polyphosphates (PP-InsPy) represent a novel group of secondary messengers that regulate diverse important cellular processes, including signal transduction, vesicle trafficking and apoptosis. Recently, it…
(more)
▼ Diphosphoinositol polyphosphates (PP-InsPy) represent a novel group of secondary messengers that regulate diverse important cellular processes, including signal transduction, vesicle trafficking and apoptosis. Recently, it has been reported that PP-InsPy phosphorylate proteins in a process known as protein pyrophosphorylation. This new type of posttranslational modification occurs in vitro, but it is still unclear if it occurs also in vivo. The concentration of PP-InsPy in cells is very low which makes their isolation from biological sources difficult. PP-InsPy have been prepared enzymatically. However, this method does not permit to obtain large amount of material necessary for biological studies. Additionally, it is not suitable for the preparation of non-natural isomers and the stereochemistry of the synthesized molecules cannot be assigned. Therefore, an efficient method to prepare a scalable amount of PP-InsPy is essential to study the structure and functions of PP-InsPy. The preparation of PP-InsPy by chemical synthesis offers the best opportunities to prepare a scalable amount of material with known stereochemistry. Additionally, this method can provide the access to several non-natural derivatives that can be used as chemical tools to study the metabolism of PP-InsPy. Different syntheses of enantiomerically pure inositol polyphosphates have been reported, but PP-InsPy are not commercially available and the quality of earlier preparations has been called into question. Asymmetric phosphorylation is an outstanding way to introduce a phosphate group in a specific position in the structure of myo-inositol. We will report a novel total synthesis of unsymmetric diphosphoinositol polyphosphates using a C2-symmetric phosphoramidite to desymmetrize different inositol derivatives. This novel phosphorylating reagent enabled us to target all four possible unsymmetric X-PP-InsP5 (1-PP-InsP5, 3-PP-InsP5, 4-PP-InsP5 and 6-PP-InsP5). Additionally, 1,5-(PP)2-InsP4 and 3,5-(PP)2-InsP4 were prepared for the first time with the same methodology. A novel synthesis of the symmetric 5-PP-InsP5 and the first total synthesis of meso 5-PPP-InsP5 will be also reported. These results represent a new approach in the envisaged total syntheses of PP-InsPy as well as the starting point for the development of efficient reagents for asymmetric phosphorylation and pyrophosphorylation. Additionally, it provided us with tools that can be used to decipher inositol related cellular signalling pathways.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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Record Details
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Capolicchio, S. (2015). Synthesis of Diphosphoinositol Polyphosphates. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/106364/1/20152470.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Capolicchio, Samanta. “Synthesis of Diphosphoinositol Polyphosphates.” 2015. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/106364/1/20152470.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Capolicchio, Samanta. “Synthesis of Diphosphoinositol Polyphosphates.” 2015. Web. 16 Jan 2021.
Vancouver:
Capolicchio S. Synthesis of Diphosphoinositol Polyphosphates. [Internet] [Thesis]. University of Zurich; 2015. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/106364/1/20152470.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Capolicchio S. Synthesis of Diphosphoinositol Polyphosphates. [Thesis]. University of Zurich; 2015. Available from: https://www.zora.uzh.ch/id/eprint/106364/1/20152470.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
12.
Unzue Lopez, Andrea.
Small Organic Molecules as Tunable Tools for Biology.
Degree: 2015, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/106367/1/20162588.pdf
► Drug discovery and development is a very challenging interdisciplinary endeavor that needs the contribution of medical doctors, biologists, chemists, X-ray crystallographers, and computer scientists, among…
(more)
▼ Drug discovery and development is a very challenging interdisciplinary endeavor that needs the contribution of medical doctors, biologists, chemists, X-ray crystallographers, and computer scientists, among many others, in order to be successful.
The first part of this Ph. D. thesis focuses on the development of EphB4 receptor tyrosine kinase inhibitors. EphB4 has been linked to angiogenesis, which involves the formation of new blood vessels supplying tumor cells with the necessary nutrients. Protein kinases play a key role in cell signaling by phosphorylating specific proteins and thus, the inhibition of their enzymatic activity by small organic molecules has been widely explored in drug design. In this work, the biological properties of an EphB4 inhibitor identified by computer simulations were improved by the synthesis of several analogues. Their binding affinities were characterized by an array of biochemical and cell based assays, concluding with the validation of one of the most promising derivatives in an in vivo cancer xenograft model.
The second part of the thesis deals with the development of novel bromodomain ligands starting from a micromolar potent in silico discovered hit. Bromodomain proteins are epigenetic readers that constitute an emerging topic in the field of drug discovery and are thus considered as very attractive targets for the development of novel therapeutic drugs. A careful, structure-based design of analogues resulted in the discovery of nanomolar potent CREBBP ligands with an unprecedented selectivity profile among the bromodomain protein family. Moreover, the screening of the synthesized analogues against several cancer cell lines revealed leukemia as a possible therapeutical application for the developed compounds.
The third aspect of this work deals with actin: a very attractive, but yet unexplored target in medicinal chemistry. Actin is a cytoskeletal protein that participates in many important cellular functions and has been linked to key pathogenic cellular processes such as angiogenesis, cell adhesion, cytokinesis and metastasis. A new computational approach to discover novel actin leads targeting the ATP binding site of actin resulted in the selection of promising compounds, which were synthesized and tested. The developed small organic molecules constitute valuable tools for the study of actin dynamics as they are able to modify the actin cytoskeleton in cells and moderately inhibit actin polymerization in vitro; thus becoming promising starting hits for the development of more potent actin binders.
The last part of this Ph.D. thesis describes the synthesis of neuroprotective compounds by the development of fumaric acid and hydroxytyrosol conjugates, for which the corresponding receptor is unknown. The biological effects of the synthesized analogues are currently under investigation, but the synergistic effect of fumaric acid and hydroxytyrosol is expected to be beneficial in the context of neuroprotection.
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Unzue Lopez, A. (2015). Small Organic Molecules as Tunable Tools for Biology. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/106367/1/20162588.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Unzue Lopez, Andrea. “Small Organic Molecules as Tunable Tools for Biology.” 2015. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/106367/1/20162588.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Unzue Lopez, Andrea. “Small Organic Molecules as Tunable Tools for Biology.” 2015. Web. 16 Jan 2021.
Vancouver:
Unzue Lopez A. Small Organic Molecules as Tunable Tools for Biology. [Internet] [Thesis]. University of Zurich; 2015. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/106367/1/20162588.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Unzue Lopez A. Small Organic Molecules as Tunable Tools for Biology. [Thesis]. University of Zurich; 2015. Available from: https://www.zora.uzh.ch/id/eprint/106367/1/20162588.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Zurich
13.
Felber, Michael.
Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core.
Degree: 2015, University of Zurich
URL: https://www.zora.uzh.ch/id/eprint/118686/1/20152444.pdf
► The application of nanoparticles (NPs) in the medical field is increasingly growing in importance. NPs such as mesoporous silica NPs, polymeric NPs, magnetic NPs, gold…
(more)
▼ The application of nanoparticles (NPs) in the medical field is increasingly growing in importance. NPs such as mesoporous silica NPs, polymeric NPs, magnetic NPs, gold NPs (AuNPs), and quantum dots (QDs) are promising candidates for the design of novel imaging, drug delivery or theranostic agents. A major challenge after administration of NPs to living organisms is the exact localization. Among the various techniques to assess the biodistribution of functional nanostructures, radiolabeling and subsequent detection of the emitted γ-photons allows for noninvasive imaging by single photon emission computed tomography (SPECT) or positron emission tomography (PET). Moreover, radiolabeling provides an accurate quantification of nanostructure localization in different organs or tissues by performing an ex vivo biodistribution.
For the 99mTc labeling of AuNPs and QDs a novel coating ligand was synthesized, containing a thiol group as an anchor for the NP surface, a spacer (e.g. polyethylene glycol PEG) and the 2,3-diaminopropionic acid (DAP) chelator for the [99mTc(CO)3]+ fragment. This ligand is multi-functional; it combines the metal chelate with conjugating functions to biological vectors in one single molecule. The concept allows coupling of any targeting function to the chelator. An example with a small molecule target for the prostate specific membrane antigen (PSMA) is given. Derivatized AuNPs and QDs can directly be labeled in one step with [99mTc(OH2)3(CO)3]+. The AuNPs in particular are highly stable in buffer and serum, a prerequisite for in vivo studies excluding misinterpretation of the biodistribution data. AuNPs with differing sizes (7 nm and 14 nm core diameter) were administered intravenously into nude NMRI mice bearing LNCaP xenografts. MicroSPECT images show for both probes rapid clearance from the blood pool via the hepatobiliary pathway. The 7 nm AuNPs revealed a significantly higher bone uptake than the 14 nm AuNPs. The high affinity towards bone mineral is further confirmed in vitro with hydroxyapatite.
In case NPs have an intrinsic property for contrast, radiolabeling automatically leads to multi-modal imaging agents. Particularly the development of NP-based dual-modality probes for magnetic resonance imaging (MRI)/PET or MRI/SPECT is intensively investigated. One of the most commonly used radionuclide for clinical SPECT imaging is 99m Tc and the labeling of Fe3O4 NPs with 99mTc was shown to be a successful strategy to obtain dual-modality imaging agents. The focus in this thesis is on the 99mTc labeling of gold containing magnetic nanomaterials (Fe3O4-Au core-shell and heterostructured Fe3O4-Au Dumbbell-like NPs). The key elements for the labeling are novel coating ligands, consisting of mono- or dithiol anchors for the gold surface, a PEG linker and various chelators for the [99mTc(CO)3]+ fragment. In a variety of labeling experiments, favorable coatings were examined and their stability tested. The findings presented herein can form the basis for the development of potential, NP-based…
Subjects/Keywords: Department of Chemistry; UZH Dissertations; 540 Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Felber, M. (2015). Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core. (Thesis). University of Zurich. Retrieved from https://www.zora.uzh.ch/id/eprint/118686/1/20152444.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Felber, Michael. “Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core.” 2015. Thesis, University of Zurich. Accessed January 16, 2021.
https://www.zora.uzh.ch/id/eprint/118686/1/20152444.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Felber, Michael. “Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core.” 2015. Web. 16 Jan 2021.
Vancouver:
Felber M. Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core. [Internet] [Thesis]. University of Zurich; 2015. [cited 2021 Jan 16].
Available from: https://www.zora.uzh.ch/id/eprint/118686/1/20152444.pdf.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Felber M. Bifunctional Ligand Systems for the Radiolabeling of Nanoparticles and Biomolecules with the fac-[99mTc(CO)3]+-Core. [Thesis]. University of Zurich; 2015. Available from: https://www.zora.uzh.ch/id/eprint/118686/1/20152444.pdf
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
14.
Peacor, Brendan.
Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:c1bcbe9f-1815-4625-8690-0143e1d4d2fa
► This dissertation focuses on the application of small molecule receptors to a fluorescent assay for the study of histone post-translational modifications, both in real-time enzyme…
(more)
▼ This dissertation focuses on the application of small molecule receptors to a fluorescent assay for the study of histone post-translational modifications, both in real-time enzyme reactions and endpoint characterization of analytes. In the first section, dynamic combinatorial
chemistry was used to generate a series of A2X receptors that varied the functionality of the X monomer. This allowed us to systematically study the contribution of pocket depth and electrostatic interactions on binding methylated lysine. We discovered that changing the location of a carboxylate increased affinity to K(Me)2, presumably through a salt bridge, while an additional carboxylate increased affinity across the entire lysine series. Additionally, formation of a deeper binding pocket saw a selectivity increase for K(Me)3 over the lower methylation states. The remaining sections describe the application of the Waters lab suite of receptors to fluorescence indicator displacement assays (IDAs). In these assays, fluorescence signal is directly proportional to the competitive binding of a histone analyte. We applied a sensor system using the receptor A2N and the fluorophore Lucigenin (LCG) to study the enzymatic dimethylation of histone H3 lysine 9 by the methyltransferase G9a. Optimization of the enzymatic buffer system established an effective methyltransferase reaction to short histone 3 peptide substrates. Applying these conditions to the fluorescent assay we are able to monitor enzymatic activity, allowing future experiments to test enzyme response to neighboring modifications in the ‘histone code’. This assay was also applied to the preliminary examination of the arginine methyltransferases, demonstrating the general applicability of the assay to the full range of enzymatic methylation reactions. With the large number of receptors previously established, we sought to develop a general discriminatory assay capable of recognizing histone modifications beyond the designed scope of the sensor. By combining the fluorescent IDA signal for four different receptors, A2B, A2D, A2N, and A2G, we were able to accurately classify thirteen different histone peptides in a single output. Each peptide had multiple modifications, including arginine methylation and lysine methylation, as well as lysine methylation and threonine phosphorylation. The classification assay was able to distinguish both the degree of modification as well as the site of the specific modifications, all based on the slight perturbations neighboring residues make on binding affinity. This assay was also preliminarily applied to the sensing of complex enzymatic reactions by performing a mock kinase experiment, in which we were able to classify distinct ‘time-point’ of enzymatic phosphorylation on two separate substrates. The final section focuses on the expansion of the target class of analytes for the combinatorial sensor array. While the previous study focused on modification-neighboring methylation events, here we describe the classification of the neutral modifications of…
Advisors/Committee Members: Peacor, Brendan, Waters, Marcey, Johnson, Jeffrey, Lawrence, David, Weeks, Kevin, Frye, Stephen.
Subjects/Keywords: Chemistry; Chemistry, Organic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Peacor, B. (2015). Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:c1bcbe9f-1815-4625-8690-0143e1d4d2fa
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Peacor, Brendan. “Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:c1bcbe9f-1815-4625-8690-0143e1d4d2fa.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Peacor, Brendan. “Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays.” 2015. Web. 16 Jan 2021.
Vancouver:
Peacor B. Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:c1bcbe9f-1815-4625-8690-0143e1d4d2fa.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Peacor B. Application of Small Molecule Receptors to the Analysis of Post-translational Modifications Using Fluorescent Indicator Displacement Assays. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:c1bcbe9f-1815-4625-8690-0143e1d4d2fa
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
15.
Blakeman, Kenion.
Development of High Pressure Mass Spectrometry for Handheld Instruments.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:820f3ab8-4f2d-419a-b07e-391cc3f141a7
► This work describes the development of microscale ion traps intended for high pressure mass spectrometry in handheld mass spectrometers. By operating at pressures approaching 1…
(more)
▼ This work describes the development of microscale ion traps intended for high pressure mass spectrometry in handheld mass spectrometers. By operating at pressures approaching 1 Torr, the major size, weight and power (SWaP) contributor, the turbopump can be eliminated. Unlike other mass analyzers, ion traps can successfully operate at higher pressures by reducing the trap size and operating at higher RF drive frequencies. HPMS was first demonstrated with helium buffer gas with volatile organic compounds (VOCs) and a ro = 500 µm cylindrical ion trap (CIT). RF frequencies up to 10 MHz minimized mass resolution loss with pressure. HPMS with nitrogen and air were then explored as field available buffer gases to eliminate helium tanks in the field, reducing instrument size and weight. Peak widths at 1.0 Torr were 0.7 Da for helium and 5 Da for nitrogen and air were observed at RF drive frequencies of 10 MHz. As peak widths widen at high pressures due to more frequent collisions, the RF frequency was increased along with a reduction in trap size to regain mass resolution. Five CITs were operated at 1 Torr in air with RF drive frequencies between 6.14 MHz to 59.44 MHz resulting in peak widths improving from 5.5 Da to 0.8 Da. Stretched length ion traps (SLITs) and 7-element CIT arrays improved sensitivity over the single element traps by factors of 6 and 7. Operating at ambient air pressures between 250 mTorr and 1.0 Torr with RF frequencies between 30 MHz and 60 MHz reduced peak widths to sub-0.6 Da. Finally, printed circuit board (PCB) and silicon ion traps were developed as alternative materials to metal ion traps. Both PCB and Si traps lower trap capacitance reducing RF power needs and improving instrument SWaP. PCB traps had a factor of two lower sensitivity and peak widths within 10% of metal traps while silicon ion traps had twice the signal intensity of metal traps and better peak widths by up to 30 %. In terms of fabrication, PCB traps can be mass produced while Si traps can be produced with higher dimensional fidelity than metal ion traps.
Advisors/Committee Members: Blakeman, Kenion, Ramsey, J. Michael, Jorgenson, James, Lockett, Matthew, Cahoon, James, Brustad, Eric.
Subjects/Keywords: Chemistry; Chemistry, Analytic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Blakeman, K. (2015). Development of High Pressure Mass Spectrometry for Handheld Instruments. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:820f3ab8-4f2d-419a-b07e-391cc3f141a7
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Blakeman, Kenion. “Development of High Pressure Mass Spectrometry for Handheld Instruments.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:820f3ab8-4f2d-419a-b07e-391cc3f141a7.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Blakeman, Kenion. “Development of High Pressure Mass Spectrometry for Handheld Instruments.” 2015. Web. 16 Jan 2021.
Vancouver:
Blakeman K. Development of High Pressure Mass Spectrometry for Handheld Instruments. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:820f3ab8-4f2d-419a-b07e-391cc3f141a7.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Blakeman K. Development of High Pressure Mass Spectrometry for Handheld Instruments. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:820f3ab8-4f2d-419a-b07e-391cc3f141a7
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
16.
Sharpe, Robert.
ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:79c97a39-bad6-48cd-9a6f-75bb32b6448d
► I. Asymmetric Synthesis of the Aminocyclitol Pactamycin, a Universal Translocation Inhibitor A concise, enantioselective synthesis of the aminocyclopentitol natural product pactamycin is presented. The critical…
(more)
▼ I. Asymmetric Synthesis of the Aminocyclitol Pactamycin, a Universal Translocation Inhibitor A concise, enantioselective synthesis of the aminocyclopentitol natural product pactamycin is presented. The critical feature of this approach was the execution of an asymmetric Mannich reaction and symmetry-breaking diketone monoreduction to assemble the C1, C2, and C7 relative stereochemistries early in the route, enabling facile construction of the remaining core functionalities. A remarkable series of serendipitous stereochemical outcomes ensued in the sequence that followed, ultimately providing the title compound in fifteen steps from the commercially available 2,4-pentanedione, constituting the shortest reported synthesis to date. The development and evolution of this synthetic strategy is thoroughly detailed, and an analysis of observed outcomes is presented. This synthesis was designed to immediately enable the facile preparation of structural analogs for the purposes of structure-activity relationship investigations. II. Preparation and Biological Evaluation of Synthetic and Polymer-Encapsulated Congeners of the Antitumor Agent Pactamycin: Insight into Functional Group Effects and Biological Activity Using the previously described total synthesis of pactamycin as a platform for synthetic diversity, twenty-five unique synthetic congeners of the natural product have been prepared to provide greater understanding into the source of pactamycin’s biological profile. Specific attention was given to the production of synthetic derivatives at the branch points of pactamycin’s unique functional groups (i.e. aniline, salicylate, and dimethylurea). In addition, the encapsulation of pactamycin and its derivatives into the PRINT© technology was demonstrated. This work has provided unprecedented access to a large number of pactamycin synthetic congeners, and subsequent in vitro analysis of the prepared compounds revealed a number of insights into the source of pactamycin’s activity. III. Inception and Development of a Global and Local Desymmetrization Approach to the Synthesis of Steroidal Alkaloids: Stereocontrolled Total Synthesis of Paspaline. An enantioselective synthesis of the indole diterpene alkaloid paspaline is described. Key features of this synthesis included the execution of both “global” and “local” desymmetrization reactions to enable expedient assembly of challenging quaternary centers in the core structure. A complete account of the conception and development of this approach is described, and an analysis of desired (and undesired) outcomes is provided. The described route affords a new conceptual blueprint for installing challenging stereocenters in this family of molecules, and the steps contained therein provide the synthetic community with complimentary disconnections in the arena of steroid natural product synthesis.
Advisors/Committee Members: Sharpe, Robert, Johnson, Jeffrey, Meek, Simon, Crimmins, Michael T., Gagne, Michel, Brookhart, Maurice.
Subjects/Keywords: Chemistry, Organic; Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Sharpe, R. (2015). ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:79c97a39-bad6-48cd-9a6f-75bb32b6448d
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Sharpe, Robert. “ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:79c97a39-bad6-48cd-9a6f-75bb32b6448d.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Sharpe, Robert. “ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE.” 2015. Web. 16 Jan 2021.
Vancouver:
Sharpe R. ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:79c97a39-bad6-48cd-9a6f-75bb32b6448d.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Sharpe R. ON THE MERITS OF STEREOSELECTIVE DESYMMETRIZATION REACTIONS IN THE ASSEMBLY OF COMPLEX NATURAL MOLECULES: THE TOTAL SYNTHESIS OF PACTAMYCIN AND PASPALINE. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:79c97a39-bad6-48cd-9a6f-75bb32b6448d
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
17.
Treadway, James.
Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:f7bdff89-494d-4a01-8c40-ccac5f087af5
► Chromatographic separations play a vital role in the separation and analysis of biological samples. Superficially porous particle have emerged as a useful particle architecture for…
(more)
▼ Chromatographic separations play a vital role in the separation and analysis of biological samples. Superficially porous particle have emerged as a useful particle architecture for liquid chromatography. These particles have received significant attention recently for the chromatographic efficiency gains that they display. Ultrahigh pressure liquid chromatography employs small particles and high pressures to also yield highly efficient separations. Increasingly, the field of chromatography had employed a combination of these two methods for creating highly efficient columns. One portion of this work details the work with micron-sized superficially porous particles for the separation of intact proteins and other large molecules. Superficially porous particles specifically tailored for the separation of large molecules are not currently commercially available in the single micron size range. One aspect of this work describes the synthetic route that was utilized to create these particles in such a small overall particle size. Another aspect of this work details an evaluation of the separation capabilities of these particles when packed into capillary columns. These columns were utilized for the separation of small molecules, peptides and proteins. Another portion of this work concerns the utilization of commercially manufactured superficially porous particles. One chapter focuses on the creation of highly efficient capillary columns packed with commercial prototype superficially porous particles. The capillary columns created in that chapter exhibit isocratic efficiencies for the separation of small molecules rivaling those seen for capillary columns packed with fully porous particles. This is the first time that such efficient separations have been demonstrated using superficially porous particles packed into capillary columns. A final section of the dissertation focuses on the comparison between commercially available fully and superficially porous particles packed into capillary columns. These particles were bonded with either conventional or charged-surface reversed-phase bondings. The separation characteristics for these columns were evaluated in terms of separating small molecules, peptides, and proteins. It was seen that both the bonded phase and the particle morphology contributed to separation differences between the columns. This work provides insight into which particle and bonding type should be pursued for future investigations.
Advisors/Committee Members: Treadway, James, Jorgenson, James, Schoenfisch, Mark H., Ramsey, J. Michael, Pielak, Gary J., Erie, Dorothy.
Subjects/Keywords: Chemistry, Analytic; Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Treadway, J. (2015). Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:f7bdff89-494d-4a01-8c40-ccac5f087af5
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Treadway, James. “Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:f7bdff89-494d-4a01-8c40-ccac5f087af5.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Treadway, James. “Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography.” 2015. Web. 16 Jan 2021.
Vancouver:
Treadway J. Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:f7bdff89-494d-4a01-8c40-ccac5f087af5.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Treadway J. Synthesis and Chromatographic Evaluation of Superficially Porous Particles for Ultrahigh Pressure Liquid Chromatography. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:f7bdff89-494d-4a01-8c40-ccac5f087af5
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
18.
Grinias, James.
Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns.
Degree: Chemistry, 2014, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:bbe9f8e7-f865-470d-85ba-ddcf19f54243
► Improving column performance remains paramount to advancing liquid chromatography (LC) technology. To that end, a series of experiments was designed to both measure and reduce…
(more)
▼ Improving column performance remains paramount to advancing liquid chromatography
(LC) technology. To that end, a series of experiments was designed to both measure and reduce
band broadening in LC columns. The main broadening mechanisms (multiple flow path
dispersion, longitudinal molecular diffusion, and resistance to mass transfer) were investigated.
Dispersion due to multiple flow paths within a packed bed were studied with a series of columns
prepared using different packing conditions. Packed column microstructure was analyzed by
confocal laser scanning microscopy (CLSM) to determine bed morphology. Column efficiency
was correlated to the bed morphology and the radial particle size distribution. Research on
longitudinal molecular diffusion focused on the validity of different stationary phase diffusion
models. Evidence was found supporting the recently proposed surface-restricted model of
surface diffusion. This result has implications affecting both gradient separations and the
calculation of the van Deemter B-term. An attempt to reduce the resistance to mass transfer term
in the stagnant mobile phase focused on the implementation of a novel sub-2 μm macroporous
silica stationary phase support. Unfortunately, the raw packing material contained a significant
number of small mesoporous fines that limited the theoretical benefits of these particles, so a
hydrodynamic chromatography (HDC) method was developed to remove the fines and reduce
the particle size distribution (PSD).
In addition to the classical on-column broadening mechanisms described above,
broadening effects due to LC operation were studied, including frictional heating and extracolumn
band broadening. When mobile phase flows over particles, frictional heating occurs.
This heating can decrease column efficiency in sub-2 μm particle-packed columns larger than 1.0
mm in diameter. Studies of frictional heating effects on columns with different dimensions,
particle types, and thermal environments were conducted to determine the impact these effects
on performance. The LC instrument can diminish efficiency due to extra-column volumes that
increase the measured peak variance. The variance contributions of the injector and connecting
tubing on a capillary UHPLC system were measured. A possible coupling effect between the
components was found that increases the tau-type (exponential decay) broadening contributions
from the injector more than theory predicts.
Advisors/Committee Members: Grinias, James, Jorgenson, James, Schoenfisch, Mark H., Ramsey, J. Michael, Lockett, Matthew, Dempsey, Jillian.
Subjects/Keywords: Chemistry, Analytic; Chemistry; College of Arts and Sciences; Department of Chemistry
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APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
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APA (6th Edition):
Grinias, J. (2014). Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:bbe9f8e7-f865-470d-85ba-ddcf19f54243
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Grinias, James. “Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns.” 2014. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:bbe9f8e7-f865-470d-85ba-ddcf19f54243.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Grinias, James. “Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns.” 2014. Web. 16 Jan 2021.
Vancouver:
Grinias J. Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns. [Internet] [Thesis]. University of North Carolina; 2014. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:bbe9f8e7-f865-470d-85ba-ddcf19f54243.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Grinias J. Characterization and Control of Band Broadening in Ultra-High Pressure Liquid Chromatography Columns. [Thesis]. University of North Carolina; 2014. Available from: https://cdr.lib.unc.edu/record/uuid:bbe9f8e7-f865-470d-85ba-ddcf19f54243
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
19.
Bertucci, Michael.
Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones.
Degree: Chemistry, 2014, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:af7e4f51-ad3f-4584-a217-3a9671bf915e
► Quorum sensing is a process of chemical communication in bacteria that enables bacteria to coordinate group function, including unified gene expression. As the quorum sensing…
(more)
▼ Quorum sensing is a process of chemical communication in bacteria that enables bacteria to coordinate group function, including unified gene expression. As the quorum sensing mechanism is in part responsible for the virulent activity of many bacteria, inhibiting the communication pathway has the potential to lead to the development of novel antibiotics. The central focus of this dissertation is the investigation of strategies for chemically activating and modifying N-acyl homoserine lactones (AHLs), the agent of chemical communication in gram-negative bacteria. Probing the inherent reactivity of the AHLs is critical to understanding their evolved function while uncovering novel modes of inhibition and tools for chemical biology. Initial studies began by utilizing small molecule thiourea and guanidine-based catalysts for accelerating ring-opening reactions of the AHL by amines. The supramolecular catalysts achieved ten and sixty-five fold increases in reaction rate, respectively, for the addition of piperidine to the characteristic α-amino-γ-butyrolactone moiety. This demonstrated the susceptibility of the chemical messengers to be activated for nucleophilic attack through appropriate arrangement of hydrogen bond donors and acceptors. Further studies on the derivatization of the AHLs continued with the development of a hydrazine-mediated transamidation reaction under aqueous conditions. Experimental evidence supports the progression of the reaction via a condensation at the α-carbon of the chemical messenger, followed by an intramolecular cyclization to cleave the AHL at the amide bond. The reaction is operable at physiological pH and is specific for the 3-oxo-AHL in the presence of other AHLs. To rapidly identify a scaffold of non-covalent interactions to increase rate of the transamidation reaction, a reactive tagging assay was developed for high-throughput screening of hydrazine-containing peptide libraries. Combinatorial libraries were synthesized with designer Boc-protected hydrazines and screened against the AHL. Colorimetric hit development was achieved through a strained-cyclooctyne functionalized dye selecting peptides that react most readily with the chemical messenger. First generation library hits were resynthesized and screened for biofilm and quorum sensing inhibition. Further library development and screening holds the potential to identify peptides sequences and structures with the greatest propensity for rapidly functionalizing the 3-oxo-AHL.
Advisors/Committee Members: Bertucci, Michael, Gagne, Michel, Waters, Marcey, Brustad, Eric, Lawrence, David, Templeton, Joseph.
Subjects/Keywords: Chemistry; Chemistry, Organic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Bertucci, M. (2014). Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:af7e4f51-ad3f-4584-a217-3a9671bf915e
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Bertucci, Michael. “Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones.” 2014. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:af7e4f51-ad3f-4584-a217-3a9671bf915e.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Bertucci, Michael. “Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones.” 2014. Web. 16 Jan 2021.
Vancouver:
Bertucci M. Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones. [Internet] [Thesis]. University of North Carolina; 2014. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:af7e4f51-ad3f-4584-a217-3a9671bf915e.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Bertucci M. Synthetic Agents for the Derivatization of N-Acyl Homoserine Lactones. [Thesis]. University of North Carolina; 2014. Available from: https://cdr.lib.unc.edu/record/uuid:af7e4f51-ad3f-4584-a217-3a9671bf915e
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
20.
Uba, Franklin.
Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics.
Degree: Chemistry, 2014, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:da41c21d-a148-4906-81fe-c4b4461f8afd
► Fluidic devices that possess structures less than 150 nm in one or two dimensions are generating great interest due to the unique properties afforded by…
(more)
▼ Fluidic devices that possess structures less than 150 nm in one or two dimensions are generating great interest due to the unique properties afforded by this size domain not accessible at the microscale. As molecules travel through nanochannels, they undergo hydrophobic and van der Waals interactions with the channel walls at a degree that depends on the size of the channel, the surface
chemistry of the wall and the debye length (governed by the ionic strength of the electrolyte solution). In this work, we report the fabrication of nanometer sized structures (nanoslits, nanochannels and nanoelectrodes) in thermoplastic and fused silica substrates for the analysis of dsNA. In the case of thermoplastics, mixed-scale micro- and nanofluidic networks were fabricated using a simple, high resolution, single-step thermal embossing process and the fluidic structures were enclosed via low temperature fusion bonding to a cover plate. Nanochannels were chemically modified and the associated electrokinetic parameters - surface charge density, zeta potential and electroosmotic flow - were evaluated. In the fused silica substrate, we developed an integrated nanosensing device comprising of a single nanochannel and two pairs of transverse electron-conducting (~50 × 50 nm) nanoelectrodes separated by a nanometer gap (nanogap) and poised at the input and output ends of the nanochannel. This device serves a foundation for a novel technique we developing for the sequencing of DNA molecule by measuring the transit time of the monomer units entering and exiting a nanochannel (5 to 50 nanochannels) after being clipped from a single polymer digested with an enzyme. Further experiments on single molecule electrophoresis will provide information on possible routes that can be adopted to engineer proper nanochannel wall
chemistry for the enhancement or reduction of solute/wall interactions.
Advisors/Committee Members: Uba, Franklin, Soper, Steven, Jorgenson, James, Murray, Royce W., Ashby, Valerie, Taylor, Anne, Lockett, Matthew.
Subjects/Keywords: Chemistry; Chemistry, Analytic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Uba, F. (2014). Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:da41c21d-a148-4906-81fe-c4b4461f8afd
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Uba, Franklin. “Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics.” 2014. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:da41c21d-a148-4906-81fe-c4b4461f8afd.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Uba, Franklin. “Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics.” 2014. Web. 16 Jan 2021.
Vancouver:
Uba F. Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics. [Internet] [Thesis]. University of North Carolina; 2014. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:da41c21d-a148-4906-81fe-c4b4461f8afd.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Uba F. Development of Nanofluidic Devices for Single-Molecule DNA Diagnostics. [Thesis]. University of North Carolina; 2014. Available from: https://cdr.lib.unc.edu/record/uuid:da41c21d-a148-4906-81fe-c4b4461f8afd
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
21.
Do, Dung.
STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN.
Degree: Chemistry, 2014, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:4fce5301-7cb1-4cfc-8b0a-8d5d6615a1c8
► I. Cu(II)-Catalyzed Aerobic Hydroperoxidation of Meldrum's Acid Derivatives and Application in Intramolecular Functionalization to Access Complex Building Blocks Aerobic hydroperoxidation of Meldrum's acid derivatives via…
(more)
▼ I. Cu(II)-Catalyzed Aerobic Hydroperoxidation of Meldrum's Acid Derivatives and Application in Intramolecular Functionalization to Access Complex Building Blocks Aerobic hydroperoxidation of Meldrum's acid derivatives via a Cu(II)-catalyzed process is presented. The mild reaction conditions are tolerant to variety of vulnerable functional groups. Au(I)-catalyzed endoperoxidations of hydroperoxyalkynes have been reported for the first time. Cleavage of the OO bond provides 1,n-diols with differentiation of the hydroxy groups. A novel research plan centered on the hydroperoxidation of designed Meldrum's acids to generally access fully substituted hemiketal-viable substrates for preparation of complex building blocks is also discussed. II. Conceptual Blueprint for a Stereoselective Heterofunctionalization of Carbonyl Compounds The glamour of a general stereoselective heterofunctionalization of carbonyl compounds encourage us to develop a novel a-heterofunctionalization of lactone. The strategy based on a highly diastereoselective Michael addition of variety of nucleophiles to readily accessible chiral alkylidene Meldrum's acid and a feasible heterofunctionalization of Meldrum's acids to access difunctionalization adducts. Those compounds have been carried on a symmetry-breaking intramolecular lactonization to reveal a new stereocenter with excellent chirality induction at carbon bearing heterofunctional group. Limited efforts provided a proof of concept for a stereoselective fluorination of lactone. III. Efforts Toward The Total Synthesis of Echinosoirin Two approaches for the construction of the echinosporin core are presented. A key strategy includes the rapid formation of the fully substituted-dihydropyran substructure via intermolecular inverse electron demand hetero Diels-Alder reaction of a chiral heterodiene. Highly diastereoselective cyclizations realized by the use of copper(II) triflate and tBu-box ligand, provided access to the dihydropyran core. The stereochemical features of this cycloaddition were previously well established and produced the dihydropyran with high diastereocontrol. An advanced intermediates diazoketone 3.54 was prepared as a single diastereomer in mulltigram-scale and will provide requisite material for further manipulations.
Advisors/Committee Members: Do, Dung, Johnson, Jeffrey, Nicewicz, David, Brookhart, Maurice, Alexanian, Erik, Templeton, Joseph.
Subjects/Keywords: Chemistry; Chemistry, Organic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Do, D. (2014). STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:4fce5301-7cb1-4cfc-8b0a-8d5d6615a1c8
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Do, Dung. “STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN.” 2014. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:4fce5301-7cb1-4cfc-8b0a-8d5d6615a1c8.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Do, Dung. “STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN.” 2014. Web. 16 Jan 2021.
Vancouver:
Do D. STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN. [Internet] [Thesis]. University of North Carolina; 2014. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:4fce5301-7cb1-4cfc-8b0a-8d5d6615a1c8.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Do D. STEREOSELECTIVE FUNCTIONALIZATION OF MELDRUM'S ACIDS AND THE EFFORTS TOWARD TOTAL SYNTHESIS OF ECHINOSPORIN. [Thesis]. University of North Carolina; 2014. Available from: https://cdr.lib.unc.edu/record/uuid:4fce5301-7cb1-4cfc-8b0a-8d5d6615a1c8
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
22.
Batz, Nicholas.
Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes.
Degree: Chemistry, 2014, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:e98451f7-4e17-4bea-bf32-f548ff861d9d
► This work describes the development of improved surface coating methods for microchip capillary electrophoresis-electrospray ionization-mass spectrometry (CE-ESI-MS) and their application for the analysis of biological…
(more)
▼ This work describes the development of improved surface coating methods for microchip capillary electrophoresis-electrospray ionization-mass spectrometry (CE-ESI-MS) and their application for the analysis of biological analytes. A new coating method based on chemical vapor deposition (CVD) of aminopropyl silane (APS) reagents is demonstrated. The method improved the efficiency of separations over previously used surface coatings while also promoting batch processing of multiple devices at once. The separation performance was quantified using a new efficiency metric based on CE theory. Microchips coated via CVD produced the most efficient liquid phase separations coupled to MS reported to date. The CVD method was found to produce a base layer well suited for subsequent modification. APS surfaces administered via CVD were modified with n-hydroxy succinimide (NHS) esters of polyethylene glycol (PEG) with varying PEG chain lengths. These coatings were found to produce highly efficient separations while offering a range of electroosmotic flow (EOF) values. PEGylation resulted in increased peak capacity and resolution as compared to APS coatings for the separation of intact proteins and digested proteins using CE-ESI microchips coupled with MS. Microfluidic CE-ESI devices with separation channels of 1 cm and 3 cm in length were coated with APS via CVD and used for high speed (HS) CE-ESI-MS of peptides and proteins. These devices were capable of CE separation times ranging from 10 s to < 1 s. To adequately sample the temporally narrow peaks generated by these devices a new MS data collection with increased data acquisition rates was developed. Both MS and tandem MS analyses were demonstrated using this high speed MS data acquisition method. The HSCE-ESI-MS separations performed on the 1 cm microchip are the fastest liquid phase separations coupled to MS reported to date. Finally, the performance limits of both the APS and PEG surface coatings were investigated. APS was applied to a CE-ESI device with a 1 m separation channel to test the ability of the CVD method to coat long channels. This device achieved > 1.4 million theoretical plates for the separation of peptide standards. A PEG surface coating was used to analyze an intact monoclonal antibody to determine structural charge variants as well as variants arising from glycosylation differences. Additionally, this PEG surface was used to inhibit the effects of sample matrix components that were deleterious to CE-ESI-MS through on-chip mobility-based sample clean-up. This approach facilitated the analysis of biological samples in matrices that would otherwise be incompatible with microchip CE-ESI-MS.
Advisors/Committee Members: Batz, Nicholas, Ramsey, J. Michael, Ramsey, J. Michael, Jorgenson, James, Allbritton, Nancy, Wightman, R. Mark, Taylor, Anne.
Subjects/Keywords: Chemistry; Chemistry, Analytic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Batz, N. (2014). Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:e98451f7-4e17-4bea-bf32-f548ff861d9d
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Batz, Nicholas. “Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes.” 2014. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:e98451f7-4e17-4bea-bf32-f548ff861d9d.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Batz, Nicholas. “Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes.” 2014. Web. 16 Jan 2021.
Vancouver:
Batz N. Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes. [Internet] [Thesis]. University of North Carolina; 2014. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:e98451f7-4e17-4bea-bf32-f548ff861d9d.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Batz N. Development and Application of Surface Coatings for Microchip Capillary Electrophoresis-Electrospray Ionization-Mass Spectrometry Analysis of Biological Analytes. [Thesis]. University of North Carolina; 2014. Available from: https://cdr.lib.unc.edu/record/uuid:e98451f7-4e17-4bea-bf32-f548ff861d9d
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

National University of Ireland – Galway
23.
Kellehan, David.
Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
.
Degree: 2012, National University of Ireland – Galway
URL: http://hdl.handle.net/10379/3405
► This thesis deals with the design, synthesis and reactivity of novel 4,4'-bisoxazoline ligands and their metal complexes; (S,S)-MePrAraBOX, (S,S)-PhPrAraBOX, (S,R)-MePrAraBOX, (S,R)-PhPrAraBOX, (S,R)-BnOAcAraBOX and (S,R)-BnOHAraBOX. Metal…
(more)
▼ This thesis deals with the design, synthesis and reactivity of novel 4,4'-bisoxazoline ligands and their metal complexes; (S,S)-MePrAraBOX, (S,S)-PhPrAraBOX, (S,R)-MePrAraBOX, (S,R)-PhPrAraBOX, (S,R)-BnOAcAraBOX and (S,R)-BnOHAraBOX. Metal complexes of these ligands have been applied to transition metal catalysed asymmetric reactions, in particular asymmetric Diels Alder, cyclopropanation and allylic alkylation reactions.
A copper(II) complex of (S,R)-PhPrAraBOX catalysed a benchmark Diels Alder reaction in up to 57% ee, the highest enantioselectivity yet achieved for a 4,4'-BOX ligand in a Diels Alder reaction. An ee of 70% was achieved with a copper(I) complex of (S,S)-MePrAraBOX in a benchmark asymmetric cyclopropanation reaction, which is also the highest enantioselectivity yet achieved for a 4,4'-BOX ligand in these reactions. The ligands were also applied to the asymmetric allylic alkylation reaction. They were the first 4,4'-BOX ligands to generate enantiocontrol in the reaction, with a palladium complex of (S,S)-MePrAraBOX producing an ee of 72%. The rationalisation of these results, in particular the results relating to the cyclopropanation reaction, are supported by computational studies carried out by colleagues in Zaragoza.
The 4,4'-bisoxazoline ligands (S,R)-BnOAcAraBOX and (S,R)-BnOHAraBOX, which contain secondary binding sites, were applied to the Diels Alder and asymmetric allylic alkylation reactions with low activity and selectivity. Ligand (S,R)-BnOHAraBOX was also applied to an asymmetric alkylation of benzaldehyde, showing low conversion and no selectivity.
Chapter One deals with the introduction of the general concepts of asymmetric synthesis and asymmetric catalysis. Chapter Two discusses the synthesis of the 4,4'-bisoxazoline ligands and the application of the metal complexes of these ligands to the asymmetric reactions. Chapter Three contains the full experimental details for the project, including spectral and analytical data.
Advisors/Committee Members: O'Leary, Patrick (advisor).
Subjects/Keywords: Bisoxazoline ligands;
Asymmetric catalysis;
Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Kellehan, D. (2012). Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
. (Thesis). National University of Ireland – Galway. Retrieved from http://hdl.handle.net/10379/3405
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Kellehan, David. “Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
.” 2012. Thesis, National University of Ireland – Galway. Accessed January 16, 2021.
http://hdl.handle.net/10379/3405.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Kellehan, David. “Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
.” 2012. Web. 16 Jan 2021.
Vancouver:
Kellehan D. Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
. [Internet] [Thesis]. National University of Ireland – Galway; 2012. [cited 2021 Jan 16].
Available from: http://hdl.handle.net/10379/3405.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Kellehan D. Synthesis and Application of Chiral AraBOX ligands for Asymmetric Catalysis
. [Thesis]. National University of Ireland – Galway; 2012. Available from: http://hdl.handle.net/10379/3405
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
24.
Gabriel, Michelle.
Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:57d3f9ac-a11a-4f7a-9ba2-e96f3833a342
► Understanding the fundamental physics of nanomaterials is critical for the advancement and rational design of new nanotechnologies. On the nanoscale, differences between individual structures, and…
(more)
▼ Understanding the fundamental physics of nanomaterials is critical for the advancement and rational design of new nanotechnologies. On the nanoscale, differences between individual structures, and even variations between different spatial locations within the same structure, can have a significant impact on the functional properties of nanomaterials and the electronic performance of nanodevices; yet much of our knowledge of nanostructure function is inferred from measurements that average over entire structures or integrate over long times. The existence of multiple conformations or structures within an ensemble, which often exhibit different dynamical behaviors, shroud the underlying dynamics, making it difficult to reach meaningful and quantitative conclusions. These limitations are overcome with the development and implementation of an ultrafast pump-probe microscopy technique. With combined spatial and temporal resolution, the microscope is capable of collecting data from individual nanostructures at various spatially distinct locations with a high throughput. Additionally, the microscope’s ability to excite an object in one location and probe it in another, allows the direct visualization of charge carrier motion and acoustic lattice motion on the nanoscale without the need for physical contact or active electrical connection. In this work, the microscope has been used to image electron diffusion in intrinsically doped silicon nanowires as well as image a combination of electron diffusion and drift in silicon nanowire devices with built-in electric fields. Additionally, to demonstrate the versatility of the microscope, it has been employed to study the insulator to metal transition and coherent acoustic phonon mode propagation in vanadium (IV) oxide (VO2) nanowires in a contactless imaging mode.
Advisors/Committee Members: Gabriel, Michelle, Papanikolas, John, Wightman, R. Mark, Ramsey, J. Michael, Cahoon, James, Atkin, Joanna.
Subjects/Keywords: Chemistry; Chemistry, Analytic; Chemistry, Physical and theoretical; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Gabriel, M. (2015). Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:57d3f9ac-a11a-4f7a-9ba2-e96f3833a342
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Gabriel, Michelle. “Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:57d3f9ac-a11a-4f7a-9ba2-e96f3833a342.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Gabriel, Michelle. “Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy.” 2015. Web. 16 Jan 2021.
Vancouver:
Gabriel M. Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:57d3f9ac-a11a-4f7a-9ba2-e96f3833a342.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Gabriel M. Imaging Ultrafast Dynamics in Nanomaterials Using Spatially-Separated Pump-Probe Microscopy. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:57d3f9ac-a11a-4f7a-9ba2-e96f3833a342
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
25.
Turner, Abigail.
Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:524c1556-dc54-49ee-9403-39d0fbb45663
► Quantification of abnormal Epidermal Growth Factor Receptor (EGFR) tyrosine kinase activity is critical to the clinical success of targeted inhibitors used to treat EGFR-dependent cancers.…
(more)
▼ Quantification of abnormal Epidermal Growth Factor Receptor (EGFR) tyrosine kinase activity is critical to the clinical success of targeted inhibitors used to treat EGFR-dependent cancers. Current selection criteria based on the presence or absence of activating mutations in the EGFR gene need to be supplemented with complementary assays which quantify EGFR biochemical activity in intact living cells. While in cellulo EGFR activity can be measured to great success in tissue cultured cells using genetically encoded reporters, such techniques are incompatible with small, highly heterogeneous tumor samples. A chemical cytometry approach to direct EGFR activity measurements is presented which consists of an in cellulo peptide reporter-based kinase assay coupled to ultrasensitive microelectrophoretic analysis. The major challenge to such a measurement is biological assay interference from off-target enzymes. A novel approach to minimizing selectivity-based assay interference and its application in single intact cells is presented.
Advisors/Committee Members: Turner, Abigail, Allbritton, Nancy, Wightman, R. Mark, Lockett, Matthew, Der, Channing, Lawrence, David.
Subjects/Keywords: Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Turner, A. (2015). Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:524c1556-dc54-49ee-9403-39d0fbb45663
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Turner, Abigail. “Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:524c1556-dc54-49ee-9403-39d0fbb45663.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Turner, Abigail. “Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis.” 2015. Web. 16 Jan 2021.
Vancouver:
Turner A. Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:524c1556-dc54-49ee-9403-39d0fbb45663.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Turner A. Epidermal Growth Factor Receptor Tyrosine Kinase Assays in Single Intact Cells Using Capillary Electrophoresis. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:524c1556-dc54-49ee-9403-39d0fbb45663
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
26.
Turlington, Christopher.
Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:57f2ae3c-469e-44bd-864d-735ee8991ad7
► The oxidation chemistry of half-sandwich iridium and rhodium complexes was explored. Iridium(Cp*) and rhodium(Cp*) complexes were prepared with various bidentate ligands and then reacted with…
(more)
▼ The oxidation
chemistry of half-sandwich iridium and rhodium complexes was explored. Iridium(Cp*) and rhodium(Cp*) complexes were prepared with various bidentate ligands and then reacted with oxygen atom transfer reagents. While oxidative degradation of the organic ligands was observed when using the oxygen atom transfer reagents iodosylbenzene and dimethyldioxirane, clean products were obtained when using a soluble derivative of iodosylbenzene, 2-tert-butylsulfonyliodosylbenzene (sPhIO). Oxidation reactions with sPhIO were typically conducted at low temperatures to increase the chance of observing reactive intermediates. It was found that the bidentate ligand 2-phenylpyridine was susceptible to insertion reactions at both metal centers. Oxygen atom insertion was observed into the rhodium-carbon bond of coordinated 2-phenylpyridine in a rhodium(Cp*) complex. Oxygen atom insertion was not observed in the analogous iridium complex; instead, an isoelectronic nitrene insertion into the iridium-carbon bond of 2-phenylpyridine occurred upon oxygen atom transfer to a coordinated nitrile ligand of the iridium(Cp*) complex. Subsequent oxygen atom transfer to the nitrene insertion compound occurred, but the iridium product could not be identified. The possible intermediacy of high-valent iridium and rhodium complexes is discussed. In addition, model iridium complexes were prepared with oxidized phenylpyridine ligands. Their reactivity suggested deactivation pathways involving the bidentate ligands of common water oxidation catalysts.
Advisors/Committee Members: Turlington, Christopher, Templeton, Joseph, Brookhart, Maurice, Meek, Simon, Lawrence, David, Schauer, Cynthia.
Subjects/Keywords: Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Turlington, C. (2015). Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:57f2ae3c-469e-44bd-864d-735ee8991ad7
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Turlington, Christopher. “Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:57f2ae3c-469e-44bd-864d-735ee8991ad7.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Turlington, Christopher. “Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium.” 2015. Web. 16 Jan 2021.
Vancouver:
Turlington C. Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:57f2ae3c-469e-44bd-864d-735ee8991ad7.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Turlington C. Oxygen Atom Transfer to Half-Sandwich Complexes of Iridium and Rhodium. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:57f2ae3c-469e-44bd-864d-735ee8991ad7
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
27.
Busan, Steven.
Frameworks for large-scale RNA structure profiling in transcriptomes and disease.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:fa2d2fe1-0129-4227-a872-ce956896a54e
► In addition to their role as intermediaries on the route to protein synthesis, RNA molecules have long been known to base-pair into complex structures that…
(more)
▼ In addition to their role as intermediaries on the route to protein synthesis, RNA molecules have long been known to base-pair into complex structures that serve specific functions. Some structured RNAs play pathogenic roles, especially in viral illnesses and repeat-expansion disorders, and disease-associated RNA structures are potential therapeutic targets. SHAPE is a well-established chemical probing strategy to interrogate RNA flexibility and obtain high-quality structure models. The recent development of an unbiased experimental approach that allows SHAPE to characterize populations of diverse RNAs using massively parallel sequencing presented a challenging data analysis problem. In this work, I apply SHAPE to study the relevance of huntingtin mRNA structure to Huntington's disease and discover that a classical CAG hairpin is likely absent or short in healthy-length transcripts. The formation of this hairpin correlates with increasing repeat length, which is a predictor of disease severity. I develop a fully-automated data analysis pipeline allowing for the extension of the SHAPE strategy to larger scales using mutational profiling (MaP), an approach that was applied to identify highly-structured elements within an HIV-1 genome. I further provide a pilot analysis of a bacterial transcriptome MaP dataset obtained in a single experiment, demonstrate the nucleotide accuracy of MaP within this large sample, and apply alignment clustering to identify conserved motifs at the genomic scale. Together, these three projects highlight the power of SHAPE to identify specific RNA structures related to human disease and the value of robust experimental design and careful analysis in large-scale sequencing studies of RNA structure.
Advisors/Committee Members: Busan, Steven, Weeks, Kevin, Pielak, Gary J., Brustad, Eric, Jarstfer, Michael, Laederach, Alain.
Subjects/Keywords: Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Busan, S. (2015). Frameworks for large-scale RNA structure profiling in transcriptomes and disease. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:fa2d2fe1-0129-4227-a872-ce956896a54e
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Busan, Steven. “Frameworks for large-scale RNA structure profiling in transcriptomes and disease.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:fa2d2fe1-0129-4227-a872-ce956896a54e.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Busan, Steven. “Frameworks for large-scale RNA structure profiling in transcriptomes and disease.” 2015. Web. 16 Jan 2021.
Vancouver:
Busan S. Frameworks for large-scale RNA structure profiling in transcriptomes and disease. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:fa2d2fe1-0129-4227-a872-ce956896a54e.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Busan S. Frameworks for large-scale RNA structure profiling in transcriptomes and disease. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:fa2d2fe1-0129-4227-a872-ce956896a54e
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
28.
Rice, Greggory.
High-throughput Experiment Driven Modeling of RNA Interactions and Structures.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:cbeb11b0-d2f3-4f68-8945-5a924e10bd59
► The higher order structure of an RNA is often essential to its biological function, modulating its interactions with ligands, protein partners, and other RNAs. Modeling…
(more)
▼ The higher order structure of an RNA is often essential to its biological function, modulating its interactions with ligands, protein partners, and other RNAs. Modeling RNA secondary structure, assessing the accuracy of RNA structural models, and discovering new functional motifs are challenging problems that are confounded by the length and complexity of the studied RNA. Improvements in structure modeling accuracy can be made by incorporating SHAPE (selective 2'-hydroxyl acylation analyzed by primer extension) and DMS (dimethyl sulfate) chemical probing data, however these models remain imperfect. In this work I apply principals of molecular modeling in interpret chemical probing experiments and create analytical and experimental tools that enable large-scale experiment-driven modeling of RNA interactions and structures. First, I use electronic structure modeling to propose a mechanism to explain the preferential reactivity of the SHAPE reagent 1M6 at nucleotides exhibiting an available open stack in folded RNAs. I also use molecular modeling at the nucleotide level to develop a model that accurately predicts the disruptive effects of SHAPE adducts on RNA tertiary structure. Second, I create a new energy potential for RNA structure prediction using information from a three-reagent SHAPE experiment that increases the accuracy of modeling accuracy from 85% to above 90% for some of the most difficult-to-predict RNA structures. Third, working collaboratively with others in the lab, I validate a new approach for melding SHAPE chemical probing with deep sequencing in a new technique termed SHAPE mutational profiling (SHAPE-MaP). The ability to quickly generate structural data for RNAs of unprecedented size using SHAPE-MaP presents a new challenge: accurately modeling large RNA secondary structures. To solve this problem I develop software, called SuperFold, which uses a windowed modeling algorithm to enable rapid secondary structure prediction and discovery of the most stable structural motifs in long RNAs. Fourth, I extend the RING-MaP experiment and analysis to enable use with random primers and applied it to the bacterial ribosome. With the improved RING-MaP experiment I am able to detect structural interaction networks within the small ribosomal subunit. Additionally, I am able to perturb those structural networks by adding the antibiotic spectinomycin. Coupled together, the work presented here will provide valuable tools that democratize RNA structure analysis and help others in the RNA community understand the role of RNA structure at new and exciting scales.
Advisors/Committee Members: Rice, Greggory, Weeks, Kevin, Pielak, Gary J., Laederach, Alain, Dokholyan, Nikolay, Lawrence, David.
Subjects/Keywords: Biochemistry; Bioinformatics; Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Rice, G. (2015). High-throughput Experiment Driven Modeling of RNA Interactions and Structures. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:cbeb11b0-d2f3-4f68-8945-5a924e10bd59
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Rice, Greggory. “High-throughput Experiment Driven Modeling of RNA Interactions and Structures.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:cbeb11b0-d2f3-4f68-8945-5a924e10bd59.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Rice, Greggory. “High-throughput Experiment Driven Modeling of RNA Interactions and Structures.” 2015. Web. 16 Jan 2021.
Vancouver:
Rice G. High-throughput Experiment Driven Modeling of RNA Interactions and Structures. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:cbeb11b0-d2f3-4f68-8945-5a924e10bd59.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Rice G. High-throughput Experiment Driven Modeling of RNA Interactions and Structures. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:cbeb11b0-d2f3-4f68-8945-5a924e10bd59
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
29.
Noucti, Njamkou.
NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:23872fdd-a25f-4d79-b4ee-c8f5dc6d3826
► Nickel–catalyzed reactions of alkene and allene π–components are reported. Through ligand–controlled selectivity, a common intermediate can be diverted to four distinct reaction pathways: (1) [2+2+2]…
(more)
▼ Nickel–catalyzed reactions of alkene and allene π–components are reported. Through ligand–controlled selectivity, a common intermediate can be diverted to four distinct reaction pathways: (1) [2+2+2] cycloaddition reactions, (2) alkenylative cyclization reactions, (3) [2+2] cycloaddition reactions, and (4) cycloisomerization reactions. The reactions utilize an inexpensive and commercially–available Ni–catalyst system with a diverse array of alkene and allene π–components to efficiently deliver stereochemically dense cycloalkanes.
Advisors/Committee Members: Noucti, Njamkou, Alexanian, Erik, Waters, Marcey, Johnson, Jeffrey, Meek, Simon, Brookhart, Maurice.
Subjects/Keywords: Chemistry, Organic; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Noucti, N. (2015). NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:23872fdd-a25f-4d79-b4ee-c8f5dc6d3826
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Noucti, Njamkou. “NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:23872fdd-a25f-4d79-b4ee-c8f5dc6d3826.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Noucti, Njamkou. “NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES.” 2015. Web. 16 Jan 2021.
Vancouver:
Noucti N. NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:23872fdd-a25f-4d79-b4ee-c8f5dc6d3826.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Noucti N. NICKEL-CATALYZED CYCLOADDITIONS OF ENE-ALLENES. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:23872fdd-a25f-4d79-b4ee-c8f5dc6d3826
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of North Carolina
30.
Wong, Hiu Ching.
Perfluoropolyether-based Electrolytes for Lithium Battary Applications.
Degree: Chemistry, 2015, University of North Carolina
URL: https://cdr.lib.unc.edu/record/uuid:f593f758-94b3-4a6e-83d0-226d0be9a1e0
► Large-scale rechargeable batteries are expected to play a key role in today's emerging sustainable energy landscape. State-of-the-art lithium-ion batteries are not only widely used in…
(more)
▼ Large-scale rechargeable batteries are expected to play a key role in today's emerging sustainable energy landscape. State-of-the-art lithium-ion batteries are not only widely used in electric vehicles, but they are currently gaining traction as backup power in aircraft and smart grid applications. In all of these cases, safety surrounding the electrolyte, an essential component of a lithium-ion battery, is a challenging limitation: the low flash points of currently used small molecule organic alkyl carbonates impose a high risk of ignition under most operating conditions. For this reason, extensive efforts are being made to develop viable nonflammable electrolytes to replace these organic solvents. Herein, we describe new classes of nonflammable liquid and solid electrolytes composed of oligomeric perfluoropolyethers. These materials are promising electrolyte alternatives due to their low glass transition temperatures, high chemical stability, capacity to dissolve lithium salts such as lithium bis(trifluoromethane)sulfonimide lithium salt, and compatibility with various common polymers such as poly(ethylene glycol). Synthetic modifications used to introduce a wide range of functional groups has created a platform of intrinsically fireproof materials that can be chemically tailored to achieve the desired physical, thermal, mechanical, and electrochemical properties for specific battery applications. Using this approach carbonate-, thiol-, allyl-, and propargyl- functionalized perfluoropolyethers were prepared from the commercially available hydroxyl-terminated PFPEs. The terminal group and molecular weight effects on the bulk properties of these materials were systematically characterized and their viability as electrolytes was evaluated. The described work ultimately paves the way towards further optimization of perfluoropolyether materials towards the development of high performance lithium- ion batteries. The interesting properties of these materials invite an extensive study into the fundamental mesoscale ion transport and the relationship between perfluoropolyether chemical structure and electrolyte electrochemical property, as well as a closer analysis into the perfluoropolyether and electrode interface. Investigation in these areas using techniques such as advanced nuclear magnetic resonance spectroscopy and transmission electron microscopy is proposed.
Advisors/Committee Members: Wong, Hiu Ching, DeSimone, Joseph M., Sheiko, Sergei, Ashby, Valerie, Murray, Royce W., Gagne, Michel.
Subjects/Keywords: Chemistry; College of Arts and Sciences; Department of Chemistry
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❌
APA ·
Chicago ·
MLA ·
Vancouver ·
CSE |
Export
to Zotero / EndNote / Reference
Manager
APA (6th Edition):
Wong, H. C. (2015). Perfluoropolyether-based Electrolytes for Lithium Battary Applications. (Thesis). University of North Carolina. Retrieved from https://cdr.lib.unc.edu/record/uuid:f593f758-94b3-4a6e-83d0-226d0be9a1e0
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Chicago Manual of Style (16th Edition):
Wong, Hiu Ching. “Perfluoropolyether-based Electrolytes for Lithium Battary Applications.” 2015. Thesis, University of North Carolina. Accessed January 16, 2021.
https://cdr.lib.unc.edu/record/uuid:f593f758-94b3-4a6e-83d0-226d0be9a1e0.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
MLA Handbook (7th Edition):
Wong, Hiu Ching. “Perfluoropolyether-based Electrolytes for Lithium Battary Applications.” 2015. Web. 16 Jan 2021.
Vancouver:
Wong HC. Perfluoropolyether-based Electrolytes for Lithium Battary Applications. [Internet] [Thesis]. University of North Carolina; 2015. [cited 2021 Jan 16].
Available from: https://cdr.lib.unc.edu/record/uuid:f593f758-94b3-4a6e-83d0-226d0be9a1e0.
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
Council of Science Editors:
Wong HC. Perfluoropolyether-based Electrolytes for Lithium Battary Applications. [Thesis]. University of North Carolina; 2015. Available from: https://cdr.lib.unc.edu/record/uuid:f593f758-94b3-4a6e-83d0-226d0be9a1e0
Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation
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