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Title: In-situ FTIR studies of the plasma glow region of catalysed non-thermal plasmas
Authors: Bin Md Ali, Abd Halim
Issue Date: 2018
Publisher: Newcastle University
Abstract: In-situ non-thermal plasma infrared transmission and reflectance cells were designed, fabricated and commissioned in order to study the non-thermal plasma (NTP)-driven reaction of methane, carbon dioxide and dinitrogen. This chemical system was chosen as a model to explore the application of in-situ FTIR spectroscopy to the study of NTP chemistry. As the choice of catalysts for NTP processes has often been made on the basis of those materials active in the analogous thermally-driven processes, the NTP experiments were supported by experiments employing a commercial, diffuse reflectance infrared Fourier transform system utilising a commercial environmental chamber that could be heated to 600˚C. Initial experiments investigated the possible reaction of CO2 and N2 in the thermal and plasma systems, the latter providing benchmark data, both quantitative and qualitative, on the NTP reduction of CO2 to CO. Experiments were also conducted on CH4 with N2, followed by studies using CH4, CO2 and N2 as the feed gas. Whilst none of the thermal experiments showed additional species other than the rotationally-excited reactants, wholly unexpected results were obtained in the NTP experiments using CH4, CO2 and N2. Nitrogen was fixed to produce both HCN and acetamide, whilst the chain oxides ketene and C5O2 were also produced along with CO and formaldehyde, and a liquid. The results were interpreted in terms of a novel, three-zone model in which the liquid products played an active part in the production of the chain oxides. SnO2 and CeO2 were also investigated with respect to possible catalytic activity, but proved inactive in both the plasma and thermal systems. Ketenes and their dimers are important reactants that find use in the production of a wide range of chemicals in a diverse range of industries including pigments, pharmaceuticals and agrochemicals and as intermediates for the paper industry. In addition, such chain oxides are known or proposed substrates for radical, nucleophilic addition and cycloaddition chemistry and hence are extremely useful chemical precursors: hence the work reported in this thesis could have significant potential implications for novel chemical synthesis. In addition to terrestrial chemistry, the production of acetamide and the chain oxides could be highly relevant to the study of the interstellar origins of life and prebiotic chemistry.
Description: PhD Thesis
Appears in Collections:School of Engineering

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