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Keywords: topological insulators optical properties synthesis
Published in RUNG: 30.09.2024; Views: 384; Downloads: 0
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Abstract: Emissions of green-house gasses have been in the forefront of scientific research in recent decades. One of the approaches towards reducing the amount of green gas CO2 in the atmosphere is its capture and storage with subsequent conversion where pure enough CO2 can be regenerated. While CO2 capture widely utilizes two mature technologies, amine absorption and cryogenic distillation, they both have significant downsides, in either cost or potential new danger to the environment. To that end an adsorption-based CO2 capture has seen quite a lot of interest in recently. Nanoporous materials have been extensively studied for this application, starting with zeolites, followed by aluminophosphates and also the new members of the porous materials group, the so called reticular porous materials. Metal-Organic Frameworks (MOFs), the first discovered reticular porous materials have shown very promising results for post combustion CO2 capture and recently also for in-door and direct air capture. MOFs are in general enough thermally stable for CO2 capture, their main weakness for wide applicability is sometimes lower selectivity for CO2 in real gas mixtures and lower stability in humid conditions. Zeolitic imidazolate frameworks (ZIFs), a subgroup of MOFs, have in recent years been extensively studied for sorption applications, also CO2, due to their superior stability and kinetics for vapour/gas adsorption if compared to carboxylate-based MOFs. While extensively studied, an overview of articles shows that most research is limited to a limited set group of frameworks, with ZIF-8 being used in more than half of ZIF papers. While ZIF-8 has successfully been prepared in water and even in solvent-free conditions, the rest of the ZIFs synthesis still heavily rely on solvothermal synthesis with formamide based solvent systems and synthesis times upwards of 5 days. Even in the case of ZIF-8, while greener synthesis approaches are available, dimethylformamide (DMF) synthesis still prevails in the cases tested for CO2 capture, mainly due to the increased CO2 uptake resulting from the synergistic contribution of the remaining DMF solvent in the pores. The goal of this thesis was to develop green synthesis approaches, both solvothermal and mechanochemical, for known ZIFs and then to extend the scope towards preparation of new ZIF materials. The goal for latter was to experimentally determine the optimal topology and functionality of ZIFs for CO2 adsorption in humid conditions. Model humid gas isotherms were developed and measured for a series of ZIFs with mostly SOD (sodalite) and RHO framework topologies and Zn and Ni as metal nodes. Finally, some novel bio-based binder materials were tested for the use with ZIFs. The sorption tests revealed than the SOD topology ZIFs have high potential for CO2 sorption applications, as the adsorption is rapid and further combination of terminally functionalised imidazoles in those frameworks drastically increases the frameworks affinity for CO2 at lower pressures. With most common 4,5- functionalised imidazole having hydrophilic functional groups, the challenge of competitive water sorption still remains. On the other hand some hydrophobic 4,5-substituted sodalite ZIFs, both with 4,5-dichloroimidazole, show excellent CO2 sorption and even complete hydrophobicity. The results led us to hypothesize that further research on ZIFs- for CO2 capture has to shift form 2 substituted sodalite frameworks to 4,5 substituted frameworks with strongly dipolar hydrophobic groups. The hydrophilic polar groups currently in use lead to issues with competitive water adsorption, due to their potential to form hydrogen bonds with water. Furthermore, some new agar and alginate based shaping methods were tested, as both potential binders are not environmentally toxic and are already used on the industrial scale world-wide for other applications.
Keywords: carbon capture, synthesis, metal-organic frameworks, zeolitic imidazolate frameworks, nanoporous materials, dissertations
Published in RUNG: 10.09.2024; Views: 684; Downloads: 19
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Abstract: Water surfaces catalyze some organic reactions more effectively, making them unique for 2D organic material synthesis. This report introduces a new synthesis method via surfactant-monolayer-assisted interfacial synthesis on water surfaces for ring-opening polymerization of pyrrole, producing distinct polypyrrole derivatives with polyacetylene backbones and ionic substitutions. The synthesis result in quasi 2D polyacetylene (q2DPA) film with enhanced charge transport behavior. We employed time-of-flight photoconductivity (TOFP) measurements using pulsed laser light of tunable wavelength for photoexcitation of the charge carriers within the q2DPA film. The charge transport was measured in the lateral direction as a function of external bias voltage ranging from 0 V to 200 V. We observed high electron mobility ({\mu}) of q2DPA reaching values of 375 cm2 V-1 s-1 at bias voltage Vb = -20V and photon energy of 3.8 eV.
Keywords: air-water interface-assisted synthesis, time-of-flight photoconductivity, 2D polymers, quasi 2D polyacetylene, q2DPA
Published in RUNG: 09.04.2024; Views: 1478; Downloads: 7
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Abstract: The Cherenkov Telescope Array (CTA) is the next generation ground-based observatory for gamma-ray astronomy at very-high energies. It will be capable of detecting gamma rays in the energy range from 20 GeV to more than 300 TeV with unprecedented precision in energy and directional reconstruction. With more than 100 telescopes of three different types it will be located in the northern hemisphere at La Palma, Spain, and in the southern at Paranal, Chile. CTA will be one of the largest astronomical infrastructures in the world with open data access and it will address questions in astronomy, astrophysics and fundamental physics in the next decades. In this presentation we will focus on the status of the CTA construction, the status of the telescope prototypes and highlight some of the physics perspectives.
Keywords: very-high-energy gamma-ray astronomy, Cherenkov Telescope Array, CTA sensitivity, gamma-ray bursts, POpulation Synthesis Theory Integrated project for very high-energy emission
Published in RUNG: 04.12.2023; Views: 1790; Downloads: 6
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Abstract: Electrochemical chlorine evolution reaction is of central importance in the chlor-alkali industry, but the chlorine evolution anode is largely limited by water oxidation side reaction and corrosion-induced performance decay in strong acids. Here we present an amorphous CoOxCly catalyst that has been deposited in situ in an acidic saline electrolyte containing Co2+ and Cl- ions to adapt to the given electrochemical condition and exhibits ~100% chlorine evolution selectivity with an overpotential of ~0.1 V at 10 mA cm−2 and high stability over 500 h. In situ spectroscopic studies and theoretical calculations reveal that the electrochemical introduction of Cl- prevents the Co sites from charging to a higher oxidation state thus suppressing the O-O bond formation for oxygen evolution. Consequently, the chlorine evolution selectivity has been enhanced on the Cl-constrained Co-O* sites via the Volmer-Heyrovsky pathway. This study provides fundamental insights into how the reactant Cl-itself can work as a promoter toward enhancing chlorine evolution in acidic brine.
Keywords: catalyst synthesis, electrocatalysis, chlorine evolution
Published in RUNG: 04.09.2023; Views: 2345; Downloads: 8
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