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Importance of the lifetime of oxygen species generated by N2O decomposition for hydrocarbon activation over Fe-silicalite

Paper ID Volume ID Publish Year Pages File Format Full-Text
48662 46517 2006 7 PDF Available
Title
Importance of the lifetime of oxygen species generated by N2O decomposition for hydrocarbon activation over Fe-silicalite
Abstract

Transient isotopic studies in the Temporal Analysis of Products (TAP) reactor evidenced a clear mechanistic regularity between methane and propane for N2O reduction over Fe-silicalite in the temperature range of 623–773 K. The lifetime of the oxygen species generated by N2O decomposition on extraframework iron sites was found to be crucial for alkane oxidation. When N2O and CH4 or C3H8 were pulsed together over Fe-silicalite, oxygen species deposited on iron sites effectively activated the hydrocarbon. However, these oxygen species become inactive for alkane oxidation if the pulses of N2O and the alkane were separated by more than 0.1 s. Transient studies have indicated that C3H8 is more efficient for N2O reduction than CH4, as expected from the facilitated activation of the CH bond upon increasing the carbon number in alkanes. The performance derived from the TAP reactor agrees well with experiments under flow conditions at ambient pressure.

Keywords
N2O decomposition; N2O reduction; Iron silicalite; Oxygen species; C3H8; CH4; Mechanism; TAP reactor
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volume 64, Issues 1–2, 18 April 2006, Pages 35–41
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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