Production of hydrogen bromide by bromine-methane reactions at elevated temperature.
Hydrogen bromide is a potentially useful intermediate for hydrogen production by electrolysis because it has a low cell potential and is extremely soluble in water. Processes have been proposed to exploit these properties, but among the important issues to be resolved is the efficiency of HBr production from hydrocarbon precursors. This investigation evaluated a fundamental facet of such a technology by studying the reaction of methane and bromine at elevated temperature to determine the yield and kinetics of HBr formation. Laboratory experimentation and computational chemistry were combined to provide a description of this reaction for possible application to reactor design at a larger scale. Experimental studies with a tubular flow reactor were used to survey a range of reactant ratios and reactor residence times at temperatures between 500 C and 800 C. At temperatures near 800 C with excess methane, conversions of bromine to HBr exceeded 90% and reaction products included solid carbon (soot) in stoichiometric amounts. At lower temperatures, HBr conversion was significantly reduced, the products included much less soot, and the formation of bromocarbon compounds was indicated qualitatively. Calculations of chemical equilibrium behavior and reaction kinetics for the experimental conditions were performed using the Sandia CHEMKIN package. An elementary multistep mechanism for the gas-phase chemistry was used together with a surface mechanism that assumed facile deposition of radical species at the reactor walls. Simulations with the laminar-flow boundary-layer code of the CHEMKIN package gave reasonable agreement with experimental data.
- Research Organization:
- Sandia National Laboratories
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC04-94AL85000
- OSTI ID:
- 918330
- Report Number(s):
- SAND2003-8061
- Country of Publication:
- United States
- Language:
- English
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