Three nickel based catalysts were prepared by the impregnation method (Ni/Al2O3 and Ni/SiO2)
and co-precipitation method (Ni/ZnO). The catalysts were characterized by XRD, ICP-OES,
BET-surface area and pore volume, SEM, TEM, TPR, NH3-TPD and in-situ XRD reduction. The
catalytic activity of the catalysts in the liquid phase hydrogenation of octanal was studied at 110
°C and 50 bar. The effect of water as a co-feed on the catalytic activity of the catalysts was also
investigated.
Generally, all the catalysts were crystalline materials. The Ni/Al2O3 and Ni/ZnO catalysts
contained NiO species that were “hard” to reduce, whereas the Ni/SiO2 catalyst was the easiest to
reduce, according to the TPR and in-situ XRD reduction studies. The total acidity (μmol
NH3/gcatal.) of the catalysts decreased in the following sequence: Ni/Al2O3 > Ni/ZnO > Ni/SiO2.
The Ni/SiO2 and Ni/ZnO catalysts had intermediate and strong acidic sites, respectively, while
the Ni/Al2O3 catalyst had weak-intermediate and strong acidic sites. The BET-surface area and
pore volume of the catalysts decreased in the following order: Ni/Al2O3 > Ni/SiO2 > Ni/ZnO.
The conversion of octanal for all the catalysts was ca. 90 %. The Ni/SiO2 and Ni/ZnO catalysts
had octanol selectivities of over 99 % and the Ni/Al2O3 catalyst had 95 % octanol selectivity. The
alumina support was observed to catalyze the formation of heavy products (C24 acetal, dioctyl
ether and 2-hexyl-1-decanol).
The water present in the feed poisoned the alumina sites that were responsible for the formation
of heavy products thereby, making the catalyst more selective (> 99 %) to octanol. For the
Ni/SiO2 catalyst the presence of water in the feed caused the octanal conversion to decrease with
time-on-stream. The deactivation of the Ni/SiO2 catalyst, when water was used as a co-feed, was
caused by the mechanical failure of the catalyst and also by the leaching of nickel metal during
the reaction. / Thesis (M.Sc.)--University of KwaZulu-Natal, Durban, 2010.
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:ukzn/oai:http://researchspace.ukzn.ac.za:10413/10633 |
| Date | January 2010 |
| Creators | Mthalane, Samkelo. |
| Contributors | Friedrich, Holger Bernhard. |
| Source Sets | South African National ETD Portal |
| Language | en_ZA |
| Detected Language | English |
| Type | Thesis |
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