Abstract
Direct nitrogen oxide decomposition (DND) is a promising alternative to the selective catalytic reduction (SCR) of nitrogen oxides for emissions control, as it eliminates the need to inject reductants such as urea/ammonia. The present study investigates the implementation of Rh-supported metal oxides for the DND reaction. Rh supported on each of PrOX, TiO2, Al2O3, and CeO2 were characterized, and we found that initially the catalytic activity on Rh/PrOX and Rh/TiO2 was very high, though it deactivated over time due to strong poisoning by adsorbed oxygen. This deactivation by oxygen poisoning was verified through in-situ DRIFTS, XPS, NEXAFS, O2-TPD measurements and density functional theory (DFT) calculations, respectively. This catalytic deactivation was positively regenerated by reductive treatments with CO or H2. This study discovers the mechanism of DND deactivation and regeneration over Rh-supported metal oxides, which will provide significant insight into further development of DND.
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