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Mechanistic Study of Partial Oxidation of Methane to Syngas Using In Situ Time‐Resolved FTIR and Microprobe Raman Spectroscopies
Author(s) -
Zheng Weng Wei,
Shu Chen Ming,
Lin Wan Hui
Publication year - 2002
Publication title -
the chemical record
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.61
H-Index - 78
eISSN - 1528-0691
pISSN - 1527-8999
DOI - 10.1002/tcr.10017
Subject(s) - syngas , partial oxidation , methane , catalysis , microprobe , rhodium , chemistry , fourier transform infrared spectroscopy , raman spectroscopy , inorganic chemistry , stoichiometry , ruthenium , chemical engineering , mineralogy , organic chemistry , physics , optics , engineering
In situ time‐resolved Fourier transform infrared (FTIR) and microprobe Raman spectroscopies were used to characterize the reaction mechanisms of the partial oxidation of methane to syngas over SiO 2 ‐ and γ‐Al 2 O 3 ‐supported rhodium and ruthenium catalysts. The interaction of both pure methane and a methane/oxygen mixture at a stoichiometric feed ratio with an oxygen‐rich catalyst surface led to the formation of CO2 and H 2 O as the primary products. For the H 2 ‐pretreated samples, the reaction mechanisms with the catalysts differ. Only Rh/SiO 2 is capable of catalyzing the direct oxidation of methane to syngas, while syngas formation over Rh/g‐Al 2 O 3 , Ru/SiO 2 , and Ru/g‐Al 2 O 3 can be achieved mainly via a combustion‐reforming scheme. The significant difference in the mechanisms for partial oxidation of methane to syngas over the catalysts can be correlated to the differences in the concentration of oxygen species (O 2− ) on the catalyst surface during the reaction, mainly due to the difference in the nature of the metals and supports. © 2002 The Japan Chemical Journal Forum and Wiley Periodicals, Inc. Chem Rec 2:102–112, 2002: Published online in Wiley InterScience (www.interscience.wiley.com) DOI 10.1002/tcr.10016