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Mechanisms and controlling characteristics of the catalytic oxidation of methane. Technical progress report, June 15, 1990--December 14, 1992
| Content Provider | United States Department of Energy Office of Scientific and Technical Information (OSTI.GOV) |
|---|---|
| Author | Klier, K. Simmons, G. W. Herman, R. G. Miller, A. C. |
| Organization | Lehigh Univ., Bethlehem, PA (United States) |
| Abstract | We have demonstrated in this work (1) that methane is readily activated at mild conditions (100{degree}C, 1 torr) over a relatively noble metal, Pd. This was observed using a stepped and kinked Pd(679) crystal (1), and other crystal faces are now being investigated to establish whether the cracking of the C-H bond of methane on Pd is structure sensitive or structure insensitive. Oxygen chemisorption is extremely structure sensitive: weakly bonded, highly reactive oxygen overlayers form on Pd(100) surface (2), while strongly bonded, moderately reactive oxygen overlayers form on Pd(111) and Pd(679). Reaction of the weakly bonded oxygen with surface carbide gives rise to CO{sub 2} over clean Pd(100) but to CO over halogen-doped Pd(100) (3--5). The effect of halogens is primarily ensemble-controlling, or oxygen-supply restricting, but long range influence of surface Cl on the strength of the Pd-O bond has also been observed (3). Because the overall chemistry of methane activation with the subsequent oxidation gives rise to the very important oxidative reforming CH{sub 4} + 1/2 O{sub 2} {yields}{sub Pd/Cl} CO + 2 H{sub 2}, Pd/Cl we plan to continue our study of this reaction in detail over Pd(100) (completed), Pd(111) (initiated), Pd(311) (initiated), Pd(110) (to be initiated), and Pd(679) (completed), without and with the halogen modifiers. |
| Sponsorship | USDOE, Washington, DC (United States) |
| Related Links | https://www.osti.gov/biblio/10108035 |
| Page Count | 13 |
| File Format | |
| DOI | 10.2172/10108035 |
| Language | English |
| Publisher Date | 1992-12-31 |
| Publisher Place | United States |
| Access Restriction | Open |
| Subject Keyword | COAL, LIGNITE, AND PEAT INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY METHANE OXIDATION CATALYSTS PROGRESS REPORT CHEMICAL ACTIVATION CHEMICAL BONDS CLEAVAGE HYDROGEN CARBON MONOXIDE FORMALDEHYDE METHANOL CARBON DIOXIDE OXYGEN AIR PARTIAL OXIDATION PROCESSES PALLADIUM CATALYTIC EFFECTS DOPED MATERIALS C1 PROCESSES CHEMICAL AND PHYSICOCHEMICAL PROPERTIES |
| Content Type | Text |
| Resource Type | Technical Report |
