Title

I. Textural/structural tuning and nanoparticle stabilization of copper-containing nanocomposite materials. II. Generation of reducing agents for automotive exhaust gas purification via the processing of hydrocarbons in a PACT (plasma and catalysis integrated technologies) reactor

Date of Completion

January 2008

Keywords

Chemistry, Inorganic|Engineering, Chemical|Engineering, Materials Science

Degree

Ph.D.

Abstract

This research consists of two parts. The first part deals with the preparation and properties of copper-containing nanocomposite materials. For studies of textural tuning, structural tuning, or material sintering, copper/aluminum and copper/zinc nanocomposites were prepared via various inorganic synthesis methods including conventional coprecipitation methods and a novel urea-gelation/thermal-modification method that produces narrow distributions of pore sizes, high surface areas, and significantly higher specific metal loadings. Solid-solid reaction analysis and differential scanning calorimetry (DSC) analysis were developed for the determination of the mixing homogeneities of the copper/aluminum nanocomposites. A sintering experiment at 250-600°C for 350 h under methanol-steam reforming conditions was carried out to compare the stability of supported Cu0 nanoparticles. The mixing homogeneities of CuO/Al2O3 nanocomposites significantly affected the thermal stability of their reduced Cu0 crystallites. Creation of relatively narrow distributions of pore sizes with relatively small major pore diameters (e.g., 3.5 nm) can also be used for the stabilization of supported Cu0 nanoparticles. The supported nanoparticles with a relatively small initial size cannot ensure good thermal stability. A "hereditary" character on the homogeneity of copper/aluminum nanocomposites was revealed. Stepwise reduction and reoxidation were studied for the structural tuning and purification of Cu-Al-O spinels with isotropic and gradual unit-cell contractions. ^ The second part of the research deals with the processing of hydrocarbons. Conversion of a model hydrocarbon (n-hexane or n-octane) in an AC discharge PACT (plasma and catalysis integrated technologies) reactor was verified to be an effective method to instantly produce reducing agents (e.g., hydrogen or/and light alkanes and alkenes), at room temperature and atmospheric pressure for automotive exhaust gas purification. Effects of electrode composition, hydrocarbon feedstock, electrode diameter, applied voltage, flow rate of carrier gas, gap size, and residence time of hydrocarbon molecules, were investigated systematically. Catalytic dehydrogenation, catalytic addition, and noncatalytic cracking reactions were discussed. Compared with space velocity, applied voltage has dominant effects on power consumption. Energy efficiency will increase as the residence time of feed molecules decreases, and decrease as applied voltage increases. ^