Document Type

Thesis

Date of Award

Fall 1-31-1994

Degree Name

Master of Science in Environmental Science - (M.S.)

Department

Chemical Engineering, Chemistry and Environmental Science

First Advisor

Joseph W. Bozzelli

Second Advisor

Richard B. Trattner

Third Advisor

Lev N. Krasnoperov

Abstract

The thermal reaction of trans-1,2-dichloroethylene (DCEE) in methane and oxygen mixtures in Ar bath gas has been studied in 10.5 mm I.D. tubular flow quartz reactors at I atmosphere pressure, isothermal temperature between 575°C and 1000°C, and times of 0.3 to 2.0 seconds.

The thermal reaction of trans-1,2-dichloroethylene in the gas phase proceeds via unimolecular HCI elimination under the reaction condition of the present experiments. The chain branching C-Cl bond fission reaction is expected to become important at the higher temperature, competing With the HCI elimination.

The decay trans- 1,2- dichloroethylene, intermediates and final product distributions varied in the absence and presence of added O2 and/or CH4. Increase in O2 concentration was observed to accelerate reagent loss in the DCEE/CH4/O2 system, especially the fuel lean and stoichiometric systems relative to the DCEE/CH4 system. Major products were C2H2, HCCCl, CH2CHCl, CH2CCl2, C6H6, CO, CO2, and HCl in the DCEE/CH4/O2 over a wide temperature range. Minor products were C2H4, CH2Cl, CH2O2, C2O2, CH3CCl3, C6H5Cl, C6H5CH3.

The extensive experimental data set will be utilized for construction and validation of a mechanism consisting of elementary reactions based on thermochemical principles, Transition State Theory and Quantum Rice-Ramsperger-Kassel (QRRK) analysis.

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