In Situ Infrared Study of G-S/L-S Adsorption and Photocatalytic Processes PDF Download

Author: Duane D. Miller
Publisher:
ISBN:
Category : Carbon dioxide
Languages : en
Pages : 438

Get Book Here

Book Description
"Coal fired power plants release large quantities of CO2 and trace amounts of SO2 into the atmosphere, affecting global warming and worldwide climate change. CO2 is a concern as a greenhouse gas in relation to global temperature raise. SO2 is a concern in environmental protection as a precursor for acid rain. The impact of CO2, SO2, and H2S on the environment demonstrate the removal process is a subject of study of great importance. Removal of these gases has been focused on the development of amine based sorbents for sequestration by the adsorption and desorption process. Fourier Transform Infrared spectroscopy (FTIR) is a powerful tool for investigating the adsorption/desorption process and structure of adsorbing molecules. The application of FTIR, coupled with ab initio quantum chemistry, can provide a direct means for understanding the interactions that occur during chemisorption. The removal of CO2 and H2S by an amine based sorbent has been studied. The hypothesis for this study is to investigate the use of polyethylene glycol (PEG) to promote tetraethylenepentamine (TEPA) CO2 and H2S removal capacity. It is thought that the use of PEG may improve the catalytic adsorption capacity through hydrogen bonding. This study used in situ FTIR and ab initio quantum chemistry to investigate the adsorption and desorption processes during CO2 and H2S capture at the molecular level. The FTIR results determine that PEG interacts with the primary amine functional groups of TEPA dispersing the adsorption sites leading to improved adsorption capacity for CO2 and H2S. Ab initio quantum chemistry determined that PEG lowers the binding energy of CO2 and H2S leading to a lower desorption temperature. Removal of the nauseous gas SO2 by an amine based sorbent is studied. The hypothesis investigated the use of 1,3-phenylenediamine low basic property for creating a reusual solid amine based sorbent for SO2 removal. It is thought that the low basic property of the aromatic amine will allow the effective SO2 adsorption and desorption at low temperature. This study used in situ FTIR spectroscopy to investigate the adsorption and desorption processes during SO2 capture. The result of this study determined that 1,3-phenylenediamine basic property allowed SO2 adsorption and desorption at 373 K, however, sorbent deactivation occurs. The in situ UV-Visible spectroscopic technique provided insight that deactivation is the result of agglomeration of 1,3-phenylenediamine. Addition of PEG prevent the agglomeration and improved the adsorption capacity of 1,2-phenylenediamine through hydrogen bonding with the primary amine functional group. Amine based sorbents have proven as an effective and economic process for the removal of CO2 and the hazardous gases H2S and SO2. Advancing knowledge in the area of amine based sorbents will improve our ability for hazardous waste management. Hazardous waste management may also be achieved by the oxidation and reduction (redox) of toxic materials. TiO2 based catalysts have the ability to oxidize a number of hazardous materials to nontoxic products where TiO2 has become the benchmark semiconductor in photo-detoxification of contaminated water. This work also investigates the photocatalytic dehydrogenation process over TiO2 based catalysts. The hypothesis investigated the relationship of the photogenerated electrons and adsorbed species during the photocatalytic dehydrogenation of 2-propanol. It is thought that the interaction of the photogenerated electrons and adsorb species may be elucidated from the reaction mechanism during the photocatalytic dehydrogenation of 2-propanol. 2-propanol is used as a model compound because it provides a simple and standard way to measure the photocatalytic activity during the gas/liquid phase reactions. This study suggest that in the presence of adsorbed H2O, the dehydrogenation process proceeded by a hydroxyl radical species while in the absence of adsorbed H2O the active species is an adsorbed ion. Au/TiO2 unique ability to generate adsorbed oxygen ions resulted in higher catalytic activity in the absence of adsorbed H2O under UV-irradiation. The reaction pathway for the photocatalytic dehydrogenation of 2-propanol is strongly dependent on the coverage of surface H2O."--Abstract.