Abstract
The N 2O decomposition mechanism on Rh/CeO 2 and Rh/γ-Al 2O 3 catalysts has been studied by pulses of isotopic N 2O and O 2 together with in situ DRIFT, XP and Raman spectroscopies. The higher catalytic activity of Rh/CeO 2 in comparison with Rh/γ-Al 2O 3 is related to the Rh–CeO 2 interaction and to the participation of the CeO 2 support in the N 2O decomposition mechanism, γ-Al 2O 3 being an inert carrier. Rhodium on Rh/γ-Al 2O 3 is reduced to Rh 0 under reaction conditions and N 2O decomposition over this catalyst mainly occurs via the Eley–Rideal mechanism. On the contrary, the ceria support interacts strongly with rhodium partially stabilizing cationic species of the noble metal during N 2O decomposition. In Rh/CeO 2, the reduced rhodium sites (by N 2O) can be reoxidized afterwards either by N 2O or by ceria oxygen, and the vacant sites created on the ceria support are then oxidized by N 2O. The active sites for N 2O chemisorption and decomposition are not only located on rhodium but also on ceria.
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