Graduation Year

2010

Document Type

Thesis

Degree

M.S.Ch.E.

Degree Granting Department

Chemical Engineering

Major Professor

John T. Wolan, Ph.D.

Co-Major Professor

Babu Joseph, Ph.D.

Committee Member

Vinay K. Gupta, Ph.D.

Keywords

silica, calcination, fixed bed reactor, biomass, diesel, aviation fuel, conversion, selectivity

Abstract

A highly selective eggshell Fischer-Tropsch catalyst has been fabricated via interaction of hydrophobic and hydrophilic molecules on thermally treated silica gel. The physical interactions of the mesoporous silica support and the effect of catalyst preparation conditions on the performance of the cobalt/SiO2 were explored. It was found that dispersion and performance of the FT cobalt/SiO2 catalyst were significantly affected by the preparation technique used. In this study we focus on two key variables: the solvent used during the precursor loading and the calcination atmosphere. Silanol groups on the silica surface and near-surface regions can alter morphology and dispersion of the supported active metals. Solvents used for precursor such as water or alcohol attach to these silanol sites in specific configurations and compete with metal salts during ion exchange and adsorption. By fine tuning the solvent attachments on heat treated silica we have fabricated a cobalt/silica catalyst with high dispersion and low metal loads. Additionally, since silica has affinity for both polar and non-polar molecule depending on the surface conditions; this property has been exploited in preparing an engineered eggshell profile. This together with simultaneous calcination/ reduction in a dynamic hydrogen environment has been shown to further enhance dispersion and reducibility. Characterization techniques including BET, XPS, XRD, H-chemisorption and FTIR were employed. Catalyst activity, product selectivity, distribution and conversion were studied using a bench scale fixed bed reactor fitted with a GC/MS instrument.

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