Introduction.- Synthesis of the Tridachiahydropyrones and their Biomimetic Precursors.- Interactions of the Tridachiahydropyrones with Model Membrane Systems: Biophysical Studies.- Investigations into the Photoprotective and Antioxidant Properties of the Tridachiahydropyrones.- Summary and Conclusions.- Experimental.- Synthesis of Alkenyl Nitriles by the Palladium-Catalysed Cyanation of Vinyl Halides with Acetone Cyanohydrin.
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This thesis addresses fundamental scientific questions such as: How are complex natural products synthesized in vivo? Can we replicate these conditions in a laboratory environment? What is the biological function of such secondary metabolites? What are the biological origins of chirality? These issues are explored in an accessible manner using a multidisciplinary approach spanning chemistry, biology and physics to investigate an interesting family of complex natural products isolated from marine molluscs - the tridachiahydropyrones. The work has achieved: Elegant biomimetic syntheses of a number of the tridachiahydropyrone compounds in vitro using organic synthesis techniques The characterization of the interactions between these compounds and a range of model membrane systems using a series of fluorescence spectroscopic studies The investigation of the antioxidant and photoprotective properties of the compounds by means of biophysical assay techniques The synthesis of tridachiahydropyrone utilizing the model membrane systems as biomimetic reaction media. (source: Nielsen Book Data) 9783319220680 20160619
Introduction.- The Hydrogen Evolution Reaction: Water Reduction Photocatalysis-Improved Niobate Nanoscroll Photocatalysts for Partial Water Splitting.- The Oxygen Evolution Reaction: Water Oxidation Photocatalysis-Photocatalytic Water Oxidation with Suspended alpha-Fe2O3 Particles - Effects of Nanoscaling.- Complete Water Splitting with Multi-Component Catalysts-Overall Water Splitting with Suspended NiO-STO nanocrystals.- Complete Water Splitting with Multi-Component Catalysts-Proposed Mechanism of Charge Transport in NiOx loaded SrTiO3 Photocatalyst for Complete Water Splitting.
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Troy Townsend's thesis explores the structure, energetics and activity of three inorganic nanocrystal photocatalysts. The goal of this work is to investigate the potential of metal oxide nanocrystals for application in photocatalytic water splitting, which could one day provide us with clean hydrogen fuel derived from water and solar energy. Specifically, Townsend's work addresses the effects of co-catalyst addition to niobium oxide nanotubes for photocatalytic water reduction to hydrogen, and the first use of iron oxide 'rust' in nanocrystal suspensions for oxygen production. In addition, Townsend studies a nickel/oxide-strontium titanate nanocomposite which can be described as one of only four nanoscale water splitting photocatalysts. He also examines the charge transport for this system. Overall, this collection of studies brings relevance to the design of inorganic nanomaterials for photocatalytic water splitting while introducing new directions for solar energy conversion. (source: Nielsen Book Data) 9783319052410 20160614
Calculating the Structural Preference of High Symmetry Clusters for PdN, AuN, and (PdAu)N
Method Development for comparing Scanning Transmission Electron Microscope Images to Theoretical Structures
A First-Principles Study of the Soft-landing of Au16 on Graphite.
In this thesis, Andrew Logsdail demonstrates that computational chemistry is a powerful tool in contemporary nanoscience, complementing experimental observations and helping guide future experiments. The aim of this particular PhD is to further our understanding of structural and compositional preferences in gold nanoparticles, as well as the compositional and chemical ordering preferences in bimetallic nanoalloys formed with other noble metals, such as palladium and platinum. Highlights include: calculations of the structural preferences and optical-response of gold nanoparticles and gold-containing nanoalloys; the design and implementation of novel numerical algorithms for the structural characterisation of gold nanoparticles from electron microscopy images; and electronic structure calculations investigating the interaction of gold nanoparticles with graphene and graphite substrates.The results presented here have significant implications for future research on the chemical and physical properties of gold-based nanoparticles and are of interest to many researchers working on experimental and theoretical aspects of nanoscience.
Book — 1 online resource : illustrations (some color)
Results and Discussion
Conclusion and Outlook
The triggered release of functional compounds from such polymeric carriers as micelles, nanoparticles or nanogels is a rapidly developing and highly versatile concept which is expected to be one of the key approaches to future therapeutics. In his thesis, Daniel Klinger highlights the approach of stimuli-responsive microgels for such applications and discusses why especially light as a trigger has an outstanding position amongst the family of conventional stimuli. Based on these considerations, the author focuses on the design, synthesis and characterization of novel photo-sensitive microgels and nanoparticles as potential materials for the loading and light-triggered release/accessibility of functional compounds. Starting from the synthesis of photo-cleavable organic building blocks and their use in the preparation of polymeric nanoparticles, continuing to the examination of their loading and release profiles, and concluding with biological in vitro studies of the final materials, Daniel Klinger's work is an excellent example of the multidisciplinary research needed for the successful development of new materials in this field and has led to a number of further publications in internationally respected journals.
In this thesis, the author investigates the chemistry and application of molecules containing urea and amide bonds. These bonds are some of the strongest known and are fundamental to biological processes. The author describes his discovery that sterically hindered ureas undergo solvolysis at room temperature under neutral conditions. This is a remarkable finding, since ureas are inert under these conditions and a general rule of chemistry is that hindered substrates are less reactive. Remarkably, the author translates these results to the correspondingly sterically hindered amides. This thesis has resulted in a number of outstanding publications in high profile journals. The unique method for breaking urea and amide bonds developed in this study is likely to have far reaching consequences for biological protein manipulation.
Pore Formation in Poly(divinylbenzene) Networks Derived from Organotellurium-Mediated Living Radical Polymerization
Extension of Living Radical Polymerization Accompanied by Phase Separation to Methacrylate- and Acrylamide-based Polymer Monoliths
Novel Monolithic Capillary Column with Well-Defined Macropores Based on Poly(styrene-co-divinylbenzene)
Fabrication of Activated Carbon Monoliths with Well-Defined Macropores Derived from Sulfonated Poly(divinylbenzene) Networks
Monolithic Electrode for Electric Double-Layer Capacitors Based on Macro/Meso/Microporous S-Containing Activated Carbon with High Surface Area
Facile Preparation of Transparent Monolithic TiO2 Gels Utilizing Chelating Ligand and Mineral Salts
Novel and Facile Preparation of Hierarchically Porous TiO2 Monoliths
Application of Hierarchically Porous Titania Monoliths to Chromatographic Separation Media
Arylene-Bridged Polysilsesquioxane Monoliths with Multi-Scale Porous Structure Prepared via Sol-Gel Process Followed by Hydrothermal Treatment
Fabrication of Macroporous SiC and SiC/C Monoliths from Arylene-Bridged Polysilsesquioxanes via Carbothermal Reduction
Hierarchically Porous Carbon Monoliths with High Surface Area from Arylene-Bridged Polysilsesquioxanes Without Thermal Activation Process
Facile Preparation of Monolithic LiFePO4/Carbon Composites with Well-Defined Macropores for Li-ion Battery
This thesis focuses on porous monolithic materials that are not in the forms of particles, fibers, or films. In particular, the synthetic strategy of porous monolithic materials via the sol-gel method accompanied by phase separation, which is characterized as the non-templating method for tailoring well-defined macropores, is described from the basics to actual synthesis. Porous materials are attracting more and more attention in various fields such as electronics, energy storage, catalysis, sensing, adsorbents, biomedical science, and separation science. To date, many efforts have been made to synthesize porous materials in various chemical compositions--organics, inorganics including metals, glasses and ceramics, and organic-inorganic hybrids. Also demonstrated in this thesis are the potential applications of synthesized porous monolithic materials to separation media as well as to electrodes for electric double-layer capacitors (EDLCs) and Li-ion batteries (LIBs). This work is ideal for graduate students in materials science and is also useful to engineers or scientists seeking basic knowledge of porous monolithic materials.
The Tight-Binding Approach and the Resulting Electronic Structure
Angle-Resolved Photoemission Spectroscopy
Electronic Raman Spectroscopy
This thesis presents the theory of three key elements of optical spectroscopy of the electronic excitations in bilayer graphene: angle-resolved photoemission spectroscopy (ARPES), visible range Raman spectroscopy, and far-infrared (FIR) magneto-spectroscopy. Bilayer graphene (BLG) is an atomic two-dimensional crystal consisting of two honeycomb monolayers of carbon, arranged according to Bernal stacking. The unperturbed BLG has a unique band structure, which features chiral states of electrons with a characteristic Berry phase of 2$\pi$, and it has versatile properties which can be controlled by an externally applied transverse electric field and strain. It is shown in this work how ARPES of BLG can be used to obtain direct information about the chirality of electron states in the crystal. The author goes on to describe the influence of the interlayer asymmetry, which opens a gap in BLG, on ARPES and on FIR spectra in a strong magnetic field. Finally, he presents a comprehensive theory of inelastic Raman scattering resulting in the electron-hole excitations in bilayer graphene, at zero and quantizing magnetic fields. This predicts their polarization properties and peculiar selection rules in terms of the inter-Landau-level transitions.