Date of Award
2001
Document Type
Dissertation - Restricted
Degree Name
Doctor of Philosophy (PhD)
Department
Mechanical Engineering
First Advisor
Brower, William E.
Second Advisor
Fournelle, Raymond
Third Advisor
Stango, Robert
Abstract
Using a flow reactor, amorphous mechanically alloyed NiZr and NiPtZr powders milled in 1 × 10-6 Torr vacuum were studied as potential catalysts for the NO decomposition and Fischer-Tropsch reactions. A commercial Ni/SiO2 -Al2 O3 catalyst was tested under the same conditions and used as a standard for comparison. Material characterization of the catalysts in the as-received and after reaction conditions was achieved using B.E.T., CO chemisorption, TGA, XRD, SEM, and TEM. The TOF's of the mechanically alloyed Ni 55 Zr45 and Ni49 PtZr 50 catalysts for the NO decomposition reaction at a reaction temperature of 673 K were two orders of magnitude greater than the commercial Ni/SiO 2 -Al2 O3 catalyst. The high activity of the mechanically alloyed catalysts for the NO decomposition reaction is believed to be due to an increase in the number of active sites, which occurred when the catalysts were exposed to reaction conditions. For the Fischer-Tropseh reaction, the most significant result was the selectivity of the mechanically alloyed NiZr and NiPtZr towards alkenes, compared to the commercial Ni/SiO 2 -Al 2 O3 catalyst, which did not produce any alkenes. Fischer-Tropsch activity results for both the mechanically alloyed NiZr and NiPtZr catalysts showed the TOF to be an order of magnitude greater than the commercial Ni/SiO 2 -Al2 O3 catalyst. The high activity of the mechanically alloyed NiZr and NiPtZr catalysts was attributed to a strong metal support interaction between crystalline Ni-containing compounds and ZrOx , which formed during exposure to isothermal reaction conditions. The transformation of the mechanically alloyed catalysts into crystalline Ni/NiZr and ZrO x also affected the selectivity, resulting in a shift towards the production of primarily methane.