By W G Frankenberg
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Extra info for Advances in Catalysis and Related Subjects, Volume 13
ACTIVITYPATTERNS IN CATALYTIC REACTIONS Another approach to the relationship between electronic structure and catalysis has been the search for catalytic activity patterns based on electron configuration and semiconductor type. The first of these patterns to be established was in nitrous oxide decomposition (69-71), as illustrated in Fig. 8. 8. The relative activity of oxides for the decomposition of nitrous oxide, showing the temperature a t which reaction first becomes appreciable. three groups.
If the oxygen gas above the oxide is removed and the temperature is raised, the vacancies diffuse t o the metal-oxide interface and the activity of the surface towards oxygen adsorption a t room temperature is regenerated. Cobaltous oxide films on cobalt behave similarly to cuprous oxide. In this case heats of adsorption have been measured as far as saturation (18). The postmonolayer uptake of oxygen (the incorporation stage) is accompanied by a fall in the heat of adsorption and a tendency towards reversible chemisorption.
Except for the anomalous magnesium, however, we may note with Greaves and Linnett that the most active catalysts also correlate with the presence of cations with unpaired d-electrons, from d9 (Cu2+)down to d4 (Mn3+). But chromia ( d 3 ) is relatively inactive. The case for correlations of activity with helectron configuration has been strongly advocated by Dowden (78). There is much experimental support for this view in the field of chemisorption and catalysis on metals, and Dowden has also sought to apply similar principles to transition metal oxides.
Advances in Catalysis and Related Subjects, Volume 13 by W G Frankenberg