| Autor: |
Radhakrishnan S; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.; NMR/X-ray Platform for Convergence Research (NMRCoRe), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Smet S; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Chandran CV; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.; NMR/X-ray Platform for Convergence Research (NMRCoRe), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Sree SP; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Duerinckx K; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.; NMR/X-ray Platform for Convergence Research (NMRCoRe), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Vanbutsele G; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Martens JA; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.; NMR/X-ray Platform for Convergence Research (NMRCoRe), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium., Breynaert E; Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.; NMR/X-ray Platform for Convergence Research (NMRCoRe), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium. |
| Abstrakt: |
Selective catalytic reduction (SCR) of NO x by ammonia is one of the dominant pollution abatement technologies for near-zero NO x emission diesel engines. A crucial step in the reduction of NO x to N 2 with Cu zeolite NH 3 -SCR catalysts is the generation of a multi-electron donating active site, implying the permanent or transient dimerization of Cu ions. Cu atom mobility has been implicated by computational chemistry as a key factor in this process. This report demonstrates how variable temperature 1 H NMR reveals the Cu induced generation of sharp 1 H resonances associated with a low concentration of sites on the zeolite. The onset temperature of the appearance of these signals was found to strongly correlate with the NH 3 -SCR activity and was observed for a range of catalysts covering multiple frameworks (CHA, AEI, AFX, ERI, ERI-CHA, ERI-OFF, *BEA), with different Si/Al ratios and different Cu contents. The results point towards universal applicability of variable temperature NMR to predict the activity of a Cu-zeolite SCR catalyst. The unique relationship of a spectroscopic feature with catalytic behavior for zeolites with different structures and chemical compositions is exceptional in heterogeneous catalysis. |
