On the enhancing effect of Ce in Pd-MOR catalysts for NOxCH4-SCR: A structure-reactivity study

The effect of palladium and cerium species on the selective catalytic reduction (SCR) of NOx using methane as reductant (NOx CH4-SCR) has been investigated using Pd-HMOR and PdCe-HMOR system. The catalysts have been characterised by H-2-TPR, DRS UV-Vis, TEM/EDS and FTIR using CO and pyridine as probe molecules. The oxidation of NO and CH4-SCR catalytic tests have been conducted using monometallic and bimetallic formulations. Above 0.3 wt.% Pd, the increase in Pd loading leads to a decrease in NOx selectivity towards N-2, with the formation of N2O, and a decrease in the CH4 selectivity towards SCR, due to CH4 direct combustion. H-2-TPR and FFIR-CO studies indicate that palladium is stabilised as Pd2+ in ion-exchange position, probably in two different sites within the MOR framework. The addition of cerium to Pd-HMOR enhances its catalytic performance for NOx CH4-SCR. With 1 wt.% Ce, both NOx conversion into N-2 and CH4 selectivity towards SCR have increased. Small CeO2 clusters interacting with palladium are likely to play a major role in this catalytic reaction. The number of such species increases up to Ce loading of ca. 2 wt.%. However, above 3 wt%, NOx conversion values decrease with Ce loading, which is attributed to the formation of bulk CeO2 species not interacting with palladium. (C) 2016 Elsevier B.V. All rights reserved.