Partial oxidation of light alkanes in transition metal ion containing zeolites: Quarterly technical progress report for the period December 15, 1988--March 14, 1989

Technical Report · Sat Apr 01 04:00:00 EST 1989

DOI:https://doi.org/10.2172/6431598· OSTI ID:6431598

Klier, Kamil ^[1]; Lange, Jean- Paul ^[1]; Herman, Richard G. ^[1]

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1. Department of Chemistry, Lehigh Univ., Bethlehem, PA (United States)

Fe(II)-A zeolites have been prepared, thermally pretreated, probed with specific adsorption species such as CO and NO, and examined by diffuse reflectance spectroscopy as detailed in a previous quarterly progress report. The spectral data have been further analyzed and the species that give rise to the spectral features are assigned and discussed. Upon thermal dehydration, the Fe(II)-A zeolite exhibited consecutively hexaquo, monoaquo, and surface trigonal Fe/sup 2 +/ species. The adsorption of NO molecules proved the accessibility of the surface trigonal iron sites. Upon contact with O/sub 2/ at 700K, the ferrous ions were oxidized to ferric species. This process consumed about one oxygen atom per iron ions. The oxidized Fe(II)-A zeolite could oxidize methane to water and carbon dioxide at temperatures as low as 600K. At the same time, a fraction of the back-reduced cations was converted to amorphous iron oxide, the presence of which conferred an enhanced activity for methane oxidation to the zeolite. Extended Hueckel calculations are being performed for several model clusters in an attempt to clarify the bonding scheme, the stability, and the electronic structure of these reactive ferrous complexes, particularly of the surface trigonal and the mononitrosyl Fe/sup 2 +/ species. 29 refs., 8 figs.

• Research Organization: Lehigh Univ., Bethlehem, PA (USA)
• Sponsoring Organization: USDOE
• DOE Contract Number: FG22-86PC90526
• OSTI ID: 6431598
• Report Number(s): DOE/PC/90526-10; ON: DE89010050
• Country of Publication: United States
• Language: English

Related Subjects

08 HYDROGEN
080109* -- Hydrogen-- Production-- Partial Oxidation Processes
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
400201 -- Chemical & Physicochemical Properties
ADSORPTION
ALKANES
CARBON COMPOUNDS
CARBON DIOXIDE
CARBON OXIDES
CHALCOGENIDES
CHARGED PARTICLES
CHEMICAL REACTIONS
DEHYDRATION
DOCUMENT TYPES
ELECTRONIC STRUCTURE
ENERGY-LEVEL TRANSITIONS
HYDROCARBONS
INORGANIC ION EXCHANGERS
ION EXCHANGE MATERIALS
IONS
IRON IONS
MATERIALS
METHANE
MINERALS
NITROGEN COMPOUNDS
NITROGEN OXIDES
ORGANIC COMPOUNDS
OXIDATION
OXIDES
OXYGEN COMPOUNDS
PARTIAL OXIDATION PROCESSES
PROGRESS REPORT
REDOX REACTIONS
SORPTION
SURFACE PROPERTIES
THERMOCHEMICAL PROCESSES
ZEOLITES