EXPERIMENTAL-EVIDENCE FOR AN OXIDATION - REDUCTION-MECHANISM IN RATE OSCILLATIONS OF CATALYTIC CO OXIDATION ON PT/SIO2

In situ X-ray diffraction experiments have been conducted during rate oscillations of catalytic CO oxidation on a supported Pt catalyst, EuroPt-1. The measurements which were carried out at atmospheric pressure with flow rates of approximately 200 ml/min showed that the non-isothermal oscillations in the reaction rate were accompanied by periodic intensity variations of a Bragg peak. A Debye function analysis of beam profiles recorded at the two extrema of the oscillations revealed that the Pt catalyst undergoes a periodic oxidation and reduction during rate oscillations. The diffraction experiments are therefore considered to be the first experimental proof that the oxide model proposed originally by Sales, Turner and Maple to explain rate oscillations in the CO + O2 reaction at atmospheric pressure is in fact correct.