A Strategic NH3-Dosing Approach for the Minimization of N2O Production During NH3-SCR Reactions over Cu-SSZ-13 Catalysts
The undesired production of N 2 O during NH 3 -SCR reactions is investigated over a reference commercial Cu-CHA catalyst. Steady-state experiments performed in the 150–500 °C temperature range exhibit a bimodal trend in the N 2 O formation profile, confirming the existence of two different reaction...
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Veröffentlicht in: | Emission control science and technology (Online) 2024-12, Vol.10 (2), p.110-122 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | The undesired production of N
2
O during NH
3
-SCR reactions is investigated over a reference commercial Cu-CHA catalyst. Steady-state experiments performed in the 150–500 °C temperature range exhibit a bimodal trend in the N
2
O formation profile, confirming the existence of two different reaction mechanisms occurring at low and high temperatures. Focusing on a low-to-medium
T
-range, N
2
O production, usually ascribed to NH
4
NO
3
formation and decomposition, increases with the NO
2
/NO
x
ratio. However, an excess of NO
2
leads to a decrease in the N
2
O release due to ammonium nitrate deposition and catalyst clogging phenomena. Steady-state and dynamics experiments show the promoting effect of both NH
3
feed concentration and NH
3
storage on N
2
O production at
T
> 200 °C. Surprisingly, N
2
O decreases with increasing NH
3
/NO
x
ratio at lower temperature. A novel approach based on the strategic injection of NH
3
is also applied to mitigate the N
2
O formation while maintaining high deNO
x
activity. Remarkably, complete NO
x
conversion and ~ 11% N
2
O saving are achieved (with inlet NO
2
/NO
x
= 0–0.5) at temperatures exceeding 200 °C; in addition, a peculiar behavior is observed in the N
2
O profile, which increases and decreases when adding and removing NH
3
from the feed, respectively. Notably, the opposite trend is observed in the N
2
O profile at 200 °C. When under Standard SCR conditions, this so far unreported observation challenges the NH
4
NO
3
formation route for N
2
O and suggests the existence of different controlling phenomena at different temperature regimes: i) the Cu/redox chemistry at
T
≤ 200 °C and ii) the NH
3
storage at higher temperature, ideally up to 300 °C. |
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ISSN: | 2199-3629 2199-3637 |
DOI: | 10.1007/s40825-024-00242-7 |