dc.contributor.author |
Wong, She Tin |
en |
dc.date.accessioned |
2007-09-10T10:10:42Z |
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dc.date.available |
2007-09-10T10:10:42Z |
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dc.date.issued |
1989 |
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dc.identifier |
THESIS 89-144 |
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dc.identifier.citation |
Thesis (PhD--Chemistry)--University of Auckland, 1989 |
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dc.identifier.uri |
http://hdl.handle.net/2292/1807 |
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dc.description |
Full text is available to authenticated members of The University of Auckland only. |
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dc.description.abstract |
In this thesis, the synthesis and characterization of the transition metal loaded AlPO4-5 catalysts are described. The catalytic properties of these catalysts were studied.
The adsorption and decomposition of Mo(CO)6, Co2(CO)8, Co(CO)3 NO and Fe(CO)5 in AlPO4-5 have been followed by gravimetric and infrared techniques. Mo(CO)6, Co(CO)3 NO and Fe(CO)5 adsorbed readily in the channels of AlPO4-5 whereas a large proportion of Co2(CO)8 adsorbed on the external surface of the channels. Activation of Mo(CO)6, Co(CO)3NO and Fe(CO)5 adsorbed onto AlPO4-5 in vacuum by heating to 673K retained and decomposed only a fraction of the initially adsorbed carbonyls in AlPO4-5. The percentage retention of the initially adsorbed Co2(CO)8 however is much higher than the other three carbonyls, as a result of more effective pore mouth blocking of the externally adsorbed Co2(CO)8 and Co4(CO)12.
The carbonyl adsorption studies showed that less subcarbonyls were produced in AlPO4-5 at room temperature than in zeolites. Except for Co2(CO)8, heating the carbonyl adsorbed AlPO4-5 samples in vacuum caused decomposition to occur directly to the metal. Co2(CO)8 adsorbed on the external surface of AlPO4-5 decomposed to Co through the formation of Co4(CO)12. Zerovalent metal particles were produced after decarbonylation of the adsorbed carbonyls.
O2- was formed in AlPO4-5 when in contact with O2. O2- showed anomalous rotational behaviour at different recording temperature.
CO hydrogenation reaction was studied on these catalysts using both recirculating and flow reactor systems. For Mo-AP-5, Co-AP-5 (Co(Co)3No) and Fe-AP-5 catalysts, the results showed that they are at least as active as their corresponding zeolite catalysts. Mo-AP-5 catalyst yielded predominantly alkanes whereas Fe-AP-5 catalyst gave high yield of alkenes. Co-AP-5 (Co(CO)3NO) catalyst gave a moderately high propene yields, but the alkane yield especially that of CH4 was also high. The Co-AP-5 (Co2(Co2(CO)8)catalyst however, deactivated rapidly as the reaction time increased. The catalytic activity and selectivity of all the catalysts were correlated to the metal particle size and dispersion. |
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dc.language.iso |
en |
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dc.publisher |
ResearchSpace@Auckland |
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dc.relation.ispartof |
PhD Thesis - University of Auckland |
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dc.relation.isreferencedby |
UoA9911337414002091 |
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dc.rights |
Restricted Item. Available to authenticated members of The University of Auckland. |
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dc.rights |
Items in ResearchSpace are protected by copyright, with all rights reserved, unless otherwise indicated. |
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dc.rights.uri |
https://researchspace.auckland.ac.nz/docs/uoa-docs/rights.htm |
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dc.title |
Transition metal loaded aluminophosphate molecular sieves |
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dc.type |
Thesis |
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thesis.degree.discipline |
Chemistry |
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thesis.degree.grantor |
The University of Auckland |
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thesis.degree.level |
Doctoral |
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thesis.degree.name |
PhD |
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dc.rights.holder |
Copyright: The author |
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dc.identifier.wikidata |
Q112849006 |
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