ETD Collection

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    Fischer Tropsch synthesis over supported cobalt catalysts: effect of ethanol addition, precursors and gold doping
    (2008-06-06T10:17:09Z) Jalama, Kalala
    The effect of the addition of ethanol (2% and 6%) during the Fischer-Tröpsch (FT) synthesis has been investigated using a 10%Co/TiO2 catalyst in a stirred basket reactor (T = 220°C, P = 8 bar, H2/CO = 2). The transformation of ethanol vapour (2% and 6% in nitrogen) over the Co/TiO2 catalyst was also studied in the absence of the synthesis gas under FT reaction conditions. Ethanol was observed to be incorporated in the growing chain and was found to (i) increase the selectivity to light products, (ii) increase the olefin to paraffin ratio and (iii) significantly decrease the catalyst activity. These effects were almost completely reversed when the ethanol in the feed was removed. Thermodynamic predictions, TPR and XRD analysis have shown that cobalt metal particles were oxidised to CoO by ethanol but that re-reduction to Co metal was possible when ethanol was removed from the feed stream allowing the catalyst to recover most of its initial performance, in particular when high flow rates were used. The effect of the cobalt carboxylate chain length (C2, C5 and C9) used in the preparation of alumina supported cobalt catalysts has been studied by TPR, XRD and hydrogen chemisorption techniques. The activity and selectivity of the prepared catalysts have been evaluated for the Fischer-Tröpsch (FT) reaction in a stirred basket reactor. It is shown that for catalysts with Co content of 10 wt.% the activity increases as the carboxylate chain length increases while the selectivity towards methane and light hydrocarbons decreases with the carboxylate chain length. The catalyst prepared using cobalt acetate was found to present the highest metal-support interaction and the poorest performance for the Fischer-Tröpsch reaction. When the metal content was increased to 15 wt.% Co and 20 wt.% Co respectively, the metal-support interaction for the catalyst prepared from cobalt acetate significantly decreased making it a better catalyst for the FT reaction compared to the catalysts prepared from C5 and C9 cobalt carboxylates. The effect of the addition of Au to a Co FT catalyst supported on titania, alumina and silica respectively, has been investigated by varying the amount of Au (0.2 to 5 wt.%) added to the catalyst. The catalysts were characterized by atomic absorption spectroscopy, XRD, XPS and TPR analysis. The catalyst evaluation for the Fischer- Tröpsch reaction activity and selectivity was achieved in a fixed bed micro-reactor (H2:CO = 2; 20 bar; 220°C). Addition of Au to supported Co catalysts improved the catalyst reduction and the cobalt dispersion on the catalyst surface. The catalyst activity for the FT reaction and the methane and light product selectivity increased with Au loading in the catalyst.
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    Performance optimisation of a compression ignition engine fuelled on Ethanol
    (2006-11-14T07:57:53Z) Teise, Heinrich Richardt
    In this research project, the performance and emissions of a conventional compression ignition engine fuelled on ethanol as main fuel and dimethyl ether as ignition promoter were investigated. Tests were first conducted on diesel fuel, then on ethanol fuel with dimethyl ether and compared. All tests for both fuelling techniques were conducted at the same engine speed and injector pressure. However, engine settings with specific reference to injection timing and injector pressure were optimised to suit diesel fuel, and were left unaltered when the engine was fuelled on ethanol and dimethyl ether. The injector nozzle configuration used for diesel fuel was a standard three-hole type nozzle, whereas for ethanol fuel with dimethyl ether a standard three-hole nozzle as well as a four-hole type nozzle was used. Also investigated was the effect a catalytic converter would have on exhaust emissions, from both fuelling techniques. The performance results of ethanol/dimethyl ether fuel compared favourably to that of diesel fuel. The brake power attained for both fuelling techniques was approximately the same, however the only penalty incurred to this desired result was the simultaneous increase in the brake specific fuel consumption of ethanol/dimethyl ether fuel. The fuel conversion efficiency of ethanol/dimethyl ether fuel was also found to be lower than that of diesel fuel, this largely attributed to the difference in energy release patterns between the two fuels. The emissions results obtained showed that ethanol/dimethyl ether fuel burns cleaner, mainly due to its chemical structure containing oxygen molecules. The NOx, THC, CO and CO2 emissions, produced before the catalytic converter, of ethanol/dimethyl ether fuel were lower than those of diesel fuel. The catalytic converter further produced lower emissions, with the four-hole type nozzle producing the most desired results. In terms of catalytic converter efficiency, THC and CO emissions were more readily removed compared to NOx. In addition, virtually no smoke emissions were detected for ethanol/dimethyl ether fuel combustion.