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Methyl chloride production from methane over lanthanum-based catalysts
Simon G Podkolzin1, Eric E Stangland, Mark E Jones
1The Dow Chemical Company, Core Research and Development, Midland, MI 48674, USA.
Journal of the American Chemical Society
|February 14, 2007
Summary
Lanthanum-based catalysts selectively produce methyl chloride via methane oxidation. The mechanism involves surface reactions and activated oxygen species, differing from traditional oxidative chlorination pathways.
Area of Science:
- Catalysis
- Surface Chemistry
- Inorganic Chemistry
Background:
- Selective methyl chloride production is crucial for chemical synthesis.
- Existing oxidative chlorination mechanisms are not fully understood.
- Lanthanum-based catalysts offer potential for improved selectivity.
Purpose of the Study:
- To elucidate the mechanism of methyl chloride production using lanthanum-based catalysts.
- To investigate the roles of methane, hydrogen chloride, and oxygen in the reaction.
- To compare the proposed mechanism with known oxidative chlorination pathways.
Main Methods:
- Catalytic activity and spectroscopic measurements.
- Kinetic and flow/pulse experiments.
- Density-functional theory (DFT) calculations.
Main Results:
- Lanthanum-based catalysts, including lanthanum oxychloride and lanthanum trichloride, are active and stable.
- Methane activation occurs on the catalyst surface via oxidation-reduction reactions.
- Gas-phase oxygen is essential, activating surface chlorine to form active OCl species.
- Hydrogen chloride's role is limited to maintaining catalyst chlorination.
Conclusions:
- A novel mechanism for selective methyl chloride production is proposed, involving surface chlorine oxidation.
- The mechanism differs significantly from established oxidative chlorination pathways.
- Lanthanum-based catalysts demonstrate high activity and stability for this transformation.
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