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(2006)ThesisPoly (co iso-butyl vinyl ether-alt-maleic anhydride), an alternating copolymer, was synthesised. For this class of copolymers the formation of an electron-donor complex is invoked to explain their microstructure in which the two comonomers strictly alternate. Due to its polarity, this copolymer constitutes a potential additive for imparting hydrophilic properties to a hydrophobic matrix. In order to obtain narrow molecular weight polymers and study the relation between the molecular weight of this additive and its ability to migrate to the host polymer surface, chain transfer agents were introduced in the system and also the Reversible Addition-Fragmentation chain Transfer (RAFT) process was employed. Free radical polymerisation was first carried out to allow for a comparison with the RAFT process and kinetics of copolymerisation was studied by NIR-FTIR and 1H NMR spectroscopy in order to analyse the rate of reaction of each comonomer. Dibenzyl trithiobenzoate, 3-benzyl sulfanyl thiocarbonyl sulfanyl-propionic acid and dibenzyl trithiobenzoate were used as RAFT agents. Results demonstrate that only benzyl dithiobenzoate is able to control the molecular weight of this copolymer and decrease its polydispersity index; possible reasons laying behind this result are discussed. It was also found that, in particular in the presence of benzyl dithiobenzoate, poly(iso-butyl vinyl ether) forms. This is an unusual phenomenon considering that the free radical polymerisation affords alternating copolymers and that iso-butyl vinyl ether is a monomer that polymerises through the cationic process. Experiments were carried out in various solvents in an attempt to counteract this side-reaction, but no appreciable correlation between the properties of the solvents and the formation of homopolymer were found. Various hypothesis are considered, however it is likely that, in the conditions adopted, the presence of the RAFT agents alters the equilibrium constant of complex formation favouring the synthesis of the homopolymer. In addition to this side-reaction also inhibition of the copolymerisation reaction was at times encountered and an investigation into this phenomenon was also conducted.
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(2006)ThesisDry/CO2 reforming is one the hydrocarbon processes that recently has been interesting due to it is ability of producing a lower synthesis gas ratio (H2/CO). This synthesis gas is a highly significant product since it costs more than 50% of the total capital cost of gas to liquid (GTL) process. However, since this reaction is thermodynamically limited, higher temperature or lower pressure is required to achieve higher conversion. Typically, reaction temperatures between 1073 and 1173 K are used for catalytic dry reforming reactions. Consequently, these extreme temperatures lead to a severe carbon deposition causing a catalyst deactivation which is the major difficulty related to CO2 reforming reaction. This has pushed the efforts to be focused mainly on the development of new catalysts. In fact, dry reforming of propane is an equilibrium-limited reaction which can be shifted to the product side by removing one of the products out of the system which can be achieved using a selective membrane reactor. This research is dedicated to investigate and study the catalytic performance of dry reforming of propane over cobalt-nickel catalyst under the temperature range of 773-973 K. This bimetallic catalyst supported on δ-Al2O3 has been utilized in this research since it exhibits better activity, selectivity, and deactivation resistance than monometallic catalysts. Based on this, the primary aims of this thesis are to examine this catalyst and to study the impact of using membrane reactor. In addition, the reaction mechanism and kinetic are investigated using a fixed-bed reactor. Experimental observations have exposed that the catalyst is offering good results under this reaction. The catalysts analysis has confirmed the presence of metal oxides in the catalyst. However, only at a lower carbon dioxide to propane ratio, i.e. lower than 3.5, a carbon signal has been reported. The activation energy study indicates that the process is unlimited by diffusion. The reaction order for propane and carbon dioxide has been found to be zero and 1.17 respectively. This in turn has indicated that C3H8 activation reaction is taking place rapidly and carbon dioxide is suggested to be involved in the rate determining step. In membrane reactor operation, the production rates for H2 and CO have been reported to increase as the sweep gas flow rate increases. The co-current mode offers higher production rate and more stability than counter-current mode over the range of feed ratio. On the other hand, fixed bed reactor shows stable performance and produces more CO and H2 for both modes.