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Mechanistic studies of the catalyzed carbon gasification reactions

Thesis/Dissertation ·
OSTI ID:6859663
The catalyzed graphite hydrogenation reaction was studied employing the Etch Decoration Transmission Electron Microscope technique to view the monolayer channeling action of nickel and ruthenium catalysts. The results indicate a carbidic catalyst surface carbon reacting with surface hydrogen to form methane as the rate limiting step of the mechanism. The mechanism is compared to the methanation reaction from CO + H{sub 2} feedstocks and also to the catalytic growth of carbon filaments. A new mode of catalytic action termed tunneling was shown to exist for Pt, Ni, and Ru in the graphite hydrogenation reaction. For monolayer channeling and tunneling the overall contribution to bulk gasification is shown to be significant. A TGA technique for measuring the solubility and diffusion coefficient of carbon in metals is presented. The technique is shown to be accurate and to give quick results in comparison to other techniques. The monolayer channeling action of Pt, Cu, V{sub 2}O{sub 5}, V and Mo{sub 2}C was examined in the graphite oxidation reaction. Pt and Cu show C-C bond breakage as the rate limiting step while V, V{sub 2}O{sub 5} and Mo{sub 2}C reveal a gas-catalyst interface reaction limiting the process. V{sub 2}O{sub 5}, V and Mo{sub 2}C were also found to participate in monolayer edge recession thus forming elongated hexagon pits.
Research Organization:
State Univ. of New York, Buffalo, NY (USA)
OSTI ID:
6859663
Country of Publication:
United States
Language:
English

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