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- All Subjects: Water--Electrolysis.
- Creators: Dahm, Werner J.A
- Creators: Mujica, Vladimiro
Description
Solar energy is a promising alternative for addressing the world's current and future energy requirements in a sustainable way. Because solar irradiation is intermittent, it is necessary to store this energy in the form of a fuel so it can be used when required. The light-driven splitting of water into oxygen and hydrogen (a useful chemical fuel) is a fascinating theoretical and experimental challenge that is worth pursuing because the advance of the knowledge that it implies and the availability of water and sunlight. Inspired by natural photosynthesis and building on previous work from our laboratory, this dissertation focuses on the development of water-splitting dye-sensitized photoelectrochemical tandem cells (WSDSPETCs). The design, synthesis, and characterization of high-potential porphyrins and metal-free phthalocyanines with phosphonic anchoring groups are reported. Photocurrents measured for WSDSPETCs made with some of these dyes co-adsorbed with molecular or colloidal catalysts on TiO2 electrodes are reported as well. To guide in the design of new molecules we have used computational quantum chemistry extensively. Linear correlations between calculated frontier molecular orbital energies and redox potentials were built and tested at multiple levels of theory (from semi-empirical methods to density functional theory). Strong correlations (with r2 values > 0.99) with very good predictive abilities (rmsd < 50 mV) were found when using density functional theory (DFT) combined with a continuum solvent model. DFT was also used to aid in the elucidation of the mechanism of the thermal relaxation observed for the charge-separated state of a molecular triad that mimics the photo-induced proton coupled electron transfer of the tyrosine-histidine redox relay in the reaction center of Photosystem II. It was found that the inclusion of explicit solvent molecules, hydrogen bonded to specific sites within the molecular triad, was essential to explain the observed thermal relaxation. These results are relevant for both advancing the knowledge about natural photosynthesis and for the future design of new molecules for WSDSPETCs.
ContributorsMéndez-Hernández, Dalvin D (Author) / Moore, Ana L (Thesis advisor) / Mujica, Vladimiro (Thesis advisor) / Gust, Devens J. (Committee member) / Gould, Ian (Committee member) / Arizona State University (Publisher)
Created2014
Description
CubeSats are a newly emerging, low-cost, rapid development platform for space exploration research. They are small spacecraft with a mass and volume of up to 12 kg and 12,000 cm3, respectively. To date, CubeSats have only been flown in Low Earth Orbit (LEO), though a large number are currently being designed to be dropped off by a mother ship on Earth escape trajectories intended for Lunar and Martian flyby missions. Advancements in propulsion technologies now enable these spacecraft to achieve capture orbits around the moon and Mars, providing a wealth of scientific data at low-cost. However, the mass, volume and launch constraints of CubeSats severely limit viable propulsion options.
We present an innovative propulsion solution using energy generated by onboard photovoltaic panels to electrolyze water, thus producing combustible hydrogen and oxygen for low-thrust applications. Water has a high storage density allowing for sufficient fuel within volume constraints. Its high enthalpy of formation provides more fuel that translates into increased ∆V and vastly reduced risk for the launch vehicle. This innovative technology poses significant challenges including the design and operation of electrolyzers at ultra-cold temperatures, the efficient separation of the resultant hydrogen and oxygen gases from liquid water in a microgravity environment, as well as the effective utilization of thrust to produce desired trajectories.
Analysis of the gas combustion and flow through the nozzle using both theoretical equations and finite-volume CFD modeling suggests an expected specific impulse of 360 s. Preliminary results from AGI's Satellite Toolkit (STK) indicate that the ΔV produced by the system for an 8kg CubeSat with 6kg of propellant in a LEO orbit (370 km altitude) is sufficient for an earth escape trajectory, lunar capture orbit or even a Mars capture orbit. These results suggest a promising pathway for an in-depth study supported by laboratory experiments to characterize the strengths and weaknesses of the proposed concept.
We present an innovative propulsion solution using energy generated by onboard photovoltaic panels to electrolyze water, thus producing combustible hydrogen and oxygen for low-thrust applications. Water has a high storage density allowing for sufficient fuel within volume constraints. Its high enthalpy of formation provides more fuel that translates into increased ∆V and vastly reduced risk for the launch vehicle. This innovative technology poses significant challenges including the design and operation of electrolyzers at ultra-cold temperatures, the efficient separation of the resultant hydrogen and oxygen gases from liquid water in a microgravity environment, as well as the effective utilization of thrust to produce desired trajectories.
Analysis of the gas combustion and flow through the nozzle using both theoretical equations and finite-volume CFD modeling suggests an expected specific impulse of 360 s. Preliminary results from AGI's Satellite Toolkit (STK) indicate that the ΔV produced by the system for an 8kg CubeSat with 6kg of propellant in a LEO orbit (370 km altitude) is sufficient for an earth escape trajectory, lunar capture orbit or even a Mars capture orbit. These results suggest a promising pathway for an in-depth study supported by laboratory experiments to characterize the strengths and weaknesses of the proposed concept.
ContributorsPothamsetti, Ramana Kumar (Author) / Thangavelautham, Jekanthan (Thesis advisor) / Dahm, Werner J.A (Committee member) / Solanki, Kiran N (Committee member) / Arizona State University (Publisher)
Created2015