The Impact of Ammonium Nitrate Species on Low Temperature NOx Conversion Over Cu/CHA SCR Catalyst 2017-01-0953
Cu/CHA catalysts have been widely used in the industry, due to their desirable performance characteristics including the unmatched hydrothermal stability. While broadly recognized for their outstanding activity at or above 200°C, these catalysts may not show desired levels of NOx conversion at lower temperatures. To achieve high NOx conversions it is desirable to have NO2/NOx close to 0.5 for fast SCR. However even under such optimal gas feed conditions, sustained use of Cu/CHA below 200°C leads to ammonium nitrate formation and accumulation, resulting in the inhibition of NOx conversion.
In this contribution, the formation and decomposition of NH4NO3 on a commercial Cu/CHA catalyst have been investigated systematically. First, the impact of NH4NO3 self-inhibition on SCR activity as a function of temperature and NO2/NOx ratios was investigated through reactor testing. Second, the formation of NH4NO3 was qualitatively measured through various adsorption and model reactions as well as its decomposition reactions by the temperature-programed desorption (TPD). In addition, the transient formation and accumulation of NH4NO3 under relevant process conditions were tracked by in situ DRIFTS spectroscopy to identify its formation and accumulation mechanisms. Last, a kinetic model was built to estimate the NH4NO3 inhibition impact on NOx conversion. This work provides insights into the limiting processes and SCR reactions at low temperatures that are important for addressing future low temperature NOx conversion needs.