Abstract
As part of a comprehensive study on the reduction of COx on supported Ru catalysts we systematically investigated the dynamic interaction of CO2 with a Ru/γ-Al2O3 catalyst in a temporal analysis of products (TAP) reactor, focusing on the redox properties of the catalyst, specifically on the deposition of active oxygen (Oact) from CO2. This was investigated by exposing the pre-reduced catalyst to CO2 pulses and subsequent titration of the deposited Oact by CO pulses. CO2 is much less active for Oact deposition than O2. Reductive co-reactants reduce (CO) or increase (H2) the activity of CO2 for Oact deposition. 18O-marked CO2 pulses show facile oxygen exchange of CO2 with the catalyst, despite the inertness of the support. Based on excess effluent CO2 we conclude that surface carbonates can both build up on the surface upon interaction with CO or CO2 and also decompose upon O2 or CO2 pulsing, releasing additional CO2.
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