Graduation Year

2003

Document Type

Thesis

Degree

M.Ch.E.

Degree Granting Department

Chemical Engineering

Major Professor

John T. Wolan, Ph.D.

Co-Major Professor

Stephen E. Saddow, Ph.D.

Committee Member

Scott W. Campbell, Ph.D.

Keywords

Pd and PdO catalysts, Oxidation of streams with lean methane concentration, Semiconductor catalys supports, SiC catalyst support, Single crystal SiC

Abstract

SiC is a hard man-made material and has emerged as an excellent material for a wide range of applications which are exposed to extreme conditions such as high temperatures and harsh chemical environments. These applications range from SiC being used as an abrasive, to a refractory material, to a semiconductor material for high power and high frequency electronic devices. The properties of the material for each application is different, with the semiconductor grade material for electronic devices being the most refined. SiC, with its excellent thermal properties and high resistance to harsh chemical environments, lends itself to being an ideal support for catalyst systems. Various characterisation & analysis techniques such as Scanning Electron Microscopy (SEM), Energy Dispersive Spectroscopy (EDS), X-ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR) and Gas Chromatography (GC) are used in this thesis to investigate the suitability of single crystal SiC for high temperature catalytic systems. Low temperature oxidation of methane was used to investigate the catalytic activity of:

  • Porous and standard 4H-SiC with and without Pd
  • Porous and Standard 6H-SiC with and without Pd.
  • Nanocrystalline Beta-SiC powder with and without Pd.

Part of the samples were impregnated with Pd using Palladium Nitrate (Pd (NO3)2) which is a common precursor for Pd. Activation treatments which were investigated were oxidation and reduction. Oxidation was generally better in activating the catalyst, as was expected, since the PdO phase is known to be more active in oxidising methane. A mixed set of Pd and PdO were observed by SEM and EDS which were the main characterisation techniques used to analyze the structure of the catalysts before and after the reaction. The Beta-SiC showed by far the best activity which could be attributed to the micro-crystalline powder format in which it was used, where as all other catalysts studied here were derived from crushed wafer pieces. Type II porous 4H-SiC was another of the samples which registered impressive results, vis-à-vis catalytic activity.

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