Reaction pathways in methanol oxidation: kinetic oscillations in the copper/oxygen system View Full Text


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

1997-11

AUTHORS

H. Werner, D. Herein, G. Schulz, U. Wild, R. Schlögl

ABSTRACT

Polycrystalline copper was used as catalyst for the selective oxidation of methanol under stoichiometric reaction conditions for oxidehydrogenation. Temperature- programmed reaction spectroscopy (TPRS) revealed a broad temperature range of reactivity with two distinct maxima for the production of formaldehyde. Phase analysis with thermogravimetry (TG) and powder X-ray diffraction (XRD) under in situ conditions showed that a phase change occurred between the two maxima for formaldehyde production from bulk Cu2O to metallic copper. Strongly adsorbed methoxy and formate were detected by X-ray photoelectron spectroscopy (XPS) after prolonged catalytic use. A sub-surface oxygen species and surface OH were identified by XPS. A region of oscillatory behaviour was found in the temperature interval between 623 and 710 K. Multicomponent gas analysis of the reaction products with an ion-molecule reaction mass spectrometer (IMR-MS) allowed to derive a reaction sequence in which both methoxy and formate are necessary as surface species. The most selective state of the catalyst for oxidehydrogenation is the co-adsorption system methanol-oxygen. Oxidation of the surface by excess molecular oxygen leads to total oxidation. The catalyst is finally reduced by excess methanol into an inactive pure metallic form. Sub-surface oxygen segregates to the surface and initiates the activity again by enhancing the sticking coefficient for gas phase species. More... »

PAGES

109-119

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http://scigraph.springernature.com/pub.10.1023/a:1019076415303

DOI

http://dx.doi.org/10.1023/a:1019076415303

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