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Conversion of polychlorinated hydrocarbons and acetylene over a nickel modified shape selective zeolite catalyst

Thesis/Dissertation ·
OSTI ID:7285686
This dissertation explores the use of a bifunctional catalyst in conversion studies of low molecular weight reactants. The catalyst is a shape selective zeolite (ZSM-5) modified via addition of elemental nickel. The resultant material combines the catalytic activity of the nickel with the acidic/shape selective properties of the zeolite. The catalysts have been employed to achieve two important advances: the complete hydrodechlorination of polychlorinated molecules and the continuous conversion of acetylene to higher hydrocarbons. The hydrodechlorination conversion couples the hydrogenolysis activity of Ni with the shape selective zeolite catalytic properties to achieve complete dechlorination of polychlorinated reactants. This dechlorination has been demonstrated for compounds including trichloroethanes, trichloroethylene, C[sub 2]Cl[sub 4] and dichloromethane. The conversion products consist of a mixture of olefins, paraffins and aromatics with the stoichiometric amount of HCl. Dependent on reaction conditions the hydrocarbon product distribution can be shaped over fairly wide ranges. The hydrodechlorination process offers potential as a more environmentally acceptable disposal process for chlorinated liquid wastes in which these wastes are converted to useful fuels and HCl. The successful continuous conversion of C[sub 2]H[sub 2] to higher molecular weight olefins, paraffins and aromatics (up to C[sub 11] compounds) over the Ni modified ZSM-5 catalyst requires addition of H[sub 2]O to the reactant C[sub 2]H[sub 2] stream. The addition of H[sub 2]O results in intermediate formation of CH[sub 3]CHO which reacts with C[sub 2]H[sub 2] to produce the hydrocarbon products. These hydrocarbon products can be shaped to provide large yields of aromatics (up to 40%). The conversion process offers a new route to synthetic fuel production based on initial conversion of coal or natural gas to acetylene.
Research Organization:
Texas Univ., Arlington, TX (United States)
OSTI ID:
7285686
Country of Publication:
United States
Language:
English