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NOx storage and reduction in model lean NOx trap catalysts studied by in situ DRIFTS

Journal Article · · Applied Catalysis B

NO{sub x} storage and reduction on a model Pt/BaO/Al{sub 2}O{sub 3} catalyst was studied by means of in situ DRIFTS measurements. To examine the effect of ceria addition, experiments were also conducted using Pt/BaO/Al{sub 2}O{sub 3} to which Pt/CeO{sub 2} was added as a physical mixture in a 74:26 weight ratio. For the former catalyst, DRIFT spectra acquired during NO/O{sub 2} and NO{sub 2}/O{sub 2} storage indicated the formation of nitrite at 200 C during the initial stages of adsorption, while increasing the adsorption temperature appeared to facilitate the oxidation of nitrite to nitrate. The ceria-containing catalyst afforded similar DRIFT spectra under these conditions, although the presence of cerium nitrates was observed at 200 and 300 C, consistent with NO{sub x} storage on the ceria phase. DRIFT spectra acquired during NO{sub x} reduction in CO and CO/H{sub 2} showed that Ba nitrate species remained on the surface of both catalysts at 450 C, whereas the use of H{sub 2}-only resulted in complete removal of stored NO{sub x}. The observation of Ba carbonates when CO was present suggests that the inferior reduction efficiency of CO may arise from the formation of a crust of BaCO{sub 3} on the Ba phase, which inhibits further NO{sub x} reduction. DRIFT spectra acquired during lean-rich cycling (6.5 min lean, 1.0 min rich) with CO/H{sub 2} as the rich phase reductants revealed that a significant concentration of nitrates remained on the catalysts at the end of the rich phase. This implies that a large fraction of nitrate is not decomposed during cycling and thus cannot participate in NO{sub x} abatement through storage and regeneration.

Research Organization:
Oak Ridge National Laboratory (ORNL)
Sponsoring Organization:
ME USDOE - Office of Management, Budget, and Evaluation; ORNL work for others
DOE Contract Number:
AC05-00OR22725
OSTI ID:
962631
Journal Information:
Applied Catalysis B, Journal Name: Applied Catalysis B Journal Issue: 1-2 Vol. 91
Country of Publication:
United States
Language:
English