About this Abstract |
Meeting |
2022 TMS Annual Meeting & Exhibition
|
Symposium
|
Advances in Powder and Ceramic Materials Science
|
Presentation Title |
F-17: Participation of Nitrosamide in the Selective Catalytic Reduction of Nitrogen Oxides over Cu/SSZ-13 |
Author(s) |
Anna C.M. Getley, Furio Corà, Jasper Berry-Gair, Chu Lun Alex Leung |
On-Site Speaker (Planned) |
Anna C.M. Getley |
Abstract Scope |
Cu/SSZ-13 is a promising ceramic for the reduction of nitrogen oxides (NOx) - released from diesel exhausts - into water and nitrogen. However, feasibly incorporating this catalyst to an industrial standard requires a full understanding of the complex reaction mechanisms. This computational work utilises Density Functional Theory to calculate equilibrium geometries and activation barriers, revealing NOx reduction half-cycle pathways over Cu/SSZ-13 with nitrosamide intermediates. The results indicate that water and ammonia ligands, previously regarded as copper-bound spectator species, instead actively influence the nitrosamide dissociation in two ways. Firstly, coordination environments determine the molecular orbital binding, affecting the N-O dissociation barrier. Secondly, the reaction is facilitated by a water or ammonia shuttle molecule at higher coordination numbers, consequently indicating a mechanism shift at lower ligation, correlating to a reduced catalytic activity. We therefore propose molecular design rules, motivated by ligation control, to systematically increase deNOx efficiency over Cu/SSZ-13. |
Proceedings Inclusion? |
Planned: |
Keywords |
Ceramics, Computational Materials Science & Engineering, Environmental Effects |