The Oscillatory Behaviour of Cu-ZSM-5 Catalysts for N2O Decomposition: Investigation of Cu species by complementary techniques.

Abstract

Copper-exchanged ZSM-5 (Cu-ZSM-5) is a promising catalyst thanks to the Cu redox pair. A particular feature of this material consists in the presence of spontaneous isothermal oscillations which take place during N2O decomposition reaction, depending on the operating conditions. In the present work, a set of five Cu-ZSM-5 catalysts are synthesised by three procedures and three different copper precursor concentrations: i) wet impregnation, ii) single ion exchange, and iii) double ion exchange. Catalytic tests reveal that the ion-exchanged samples exhibit a low catalytic activity and no oscillatory behaviour, except for the twice-exchanged sample which achieves an average N2O conversion of 26% at 400 °C. Conversely, the impregnated samples reach higher levels of N2O conversion (66% for Cu5ZSM5_WI and 72% for Cu10ZSM5_WI) and demonstrate a similar oscillating pattern. Further investigations disclosed that the most active catalysts, characterised by the presence of oscillatory behaviour, have more abundant and easily reducible copper specis (ICP, EDX and H2-TPR) which interacts better with the zeolitic support (FT-IR). Catalytic tests under a long time on stream (TOS) suggest that either self-organised patterns or deterministic chaos can be achieved during the reaction, depending on the operating conditions, such as temperature and contact time.