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Applied Experimental Surface Chemistry at Solid-Liquid and Solid-Gas Interface: A UHV Study of Carbon Dioxide Sorption on Single and Composite Alkali and Alkaline Earth Metal (potassium modified magnesia) Films and Using Zeta Potential to Probe Surface Re

Posted on:2011-11-27Degree:Ph.DType:Thesis
University:Carnegie Mellon UniversityCandidate:Faruqui, DanishFull Text:PDF
GTID:2441390002454519Subject:Engineering
Abstract/Summary:PDF Full Text Request
This thesis focuses on experimental methodologies to address surface science problems at solid-liquid and solid-gas interfaces. Theoretical modeling and analysis accompanies experimental data to explain and analyze new findings obtained by experiments. This Ph.D thesis addresses problems of "surface chemistry" wherein we attempted to probe (experimentally), understand (based on theoretical analysis) and control (based on experimental results and model predictions) reaction and processes occurring at surfaces of materials of interest. The majority of general surface science problems fall in either of the two category, solid-gas (S-G) or solid-liquid (S-L) interfaces, we attempted to probe surface chemistry in each system.;At the S-L interface we develop, propose and apply an experimental methodology and theoretical modeling to both experimentally detect/track and theoretically predict the kinetics of surface reactions occurring at planar mineral-liquid interfaces. We employ an experimental capability for measuring time dependent zeta potential changes due to surface reaction kinetics at mineral-liquid interface and propose an accompanying theoretical kinetic surface reaction model. The proposed kinetic surface reaction model apart from being simpler and less expensive than existing equilibrium models on parameter estimation gives new insight into an unexplored regime of earliest (pre-equilibrium) interactions occurring after immersion of a solid in liquid media which results in non-monotonic charging of solids. Also we propose an alternate and advantageous way of equilibrium surface reaction modeling and experimentation over existing techniques based on a transformation invented in this work. We employed planar surfaces of mica, quartz, and, fused silica and studied the kinetic and equilibrium of surface reactions in liquid environments of choice.;Using several ultra high vacuum (UHV) surface science techniques we attempted to fundamentally understand and develop dry metallic sorbents for CO 2 capture (S-G interface). A candidate each from alkali (potassium) and alkaline earth (magnesium) metal were employed in the form of well developed thin film surfaces to study their CO2 adsorption, desorption characteristics under varied conditions. We studied both metal and metal oxide forms of each candidate and also designed two composite sorbents employing both metals and their oxides and further studied their characteristics using UHV techniques such as sputtering/film-deposition/TPD/XPS.
Keywords/Search Tags:Surface, UHV, Experimental, Metal, Interface, Solid-gas, Using, Solid-liquid
PDF Full Text Request
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