Applied Catalysis B: Environmental, Vol.184, 364-380, 2016
Towards optimal operation of sequential NOx storage and reduction and selective catalytic reduction
Combined NOx storage and reduction (NSR) and selective catalytic reduction (SCR) were conducted in a bench flow reactor comprising a Pt/Rh/BaO/Al2O3 lean NOx trap (LNT) catalyst and either Fe-ZSM-5 or Cu-SSZ-13 SCR catalyst. Simulated exhaust gas containing C3H6 or CO reductant was used to evaluate catalyst performance in terms of cycle-averaged NOx conversion and product selectivities over a range of feed concentrations and temperatures, and gas hourly space velocities (GHSV). Instantaneous concentration and temperature measurements reveal strong coupling of mass and energy between the LNT and SCR. The data show the importance of NH3 generation by the LNT for effective use of the downstream SCR. Operating conditions are identified that maximize utilization of the downstream SCR. A non-NH3 SCR pathway is found to be significant for Cu-SSZ-13 at intermediate temperature and high space velocity. The post-LNT NH3 to NOx ratio (ANR) correlates with the incremental NOx conversion achieved for Fe-ZSM-5, noting that ANR similar to 1 favors NH3-based standard SCR at high conversion. A reactor system productivity metric for N-2 generation (space-time yield analog) is used to rank-order the LNT + SCR systems and together with the propylene conversion are used to identify conditions giving the best performance. The combination of an overall GHSV of 135 k h(-1) and 350 degrees C feed temperature generates a SCR feed from the LNT that results in the highest incremental cycle-averaged NOx conversion in the SCR (similar to 30% with Cu-SSZ-13) and high cycle-averaged conversions of NOx (similar to 90%) and propylene (similar to 80%). The Cu-SSZ-13 out-performs the Fe-ZSM-5 catalyst under most conditions. (C) 2015 Elsevier B.V. All rights reserved.