The effect of hydrothermal aging on Mn2O3/Cu-SSZ-39 composite catalysts for selective catalytic reduction of NOx by NH3

Abstract

The latest generation of fuel-efficient engines produces exhaust at cooler temperatures, highlighting a need for enhancement in the low-temperature effectiveness of Cu-zeolite catalysts. The metal oxide/Cu-zeolite composite catalysts have demonstrated superior deNOx performance at lower temperatures compared to Cu-zeolite alone. However, the hydrothermal stability of these composite catalysts remains unexplored. In this study, we focus on the Mn2O3/Cu-SSZ-39 catalyst, chosen for its exceptional activity at low temperatures. The synergy between the nitrate groups on Mn2O3 and NH4+ ions on the Brønsted acid sites of Cu-SSZ-39 enhances NOx conversion efficiency. Nonetheless, the efficiency of Mn2O3/Cu-SSZ-39 diminishes following exposure to hydrothermal conditions at various temperatures (700 °C, 750 °C, and 800 °C), with the degradation degree intensifying at higher temperatures. Characterization studies revealed that hydrothermal treatment leads to the recrystallization of Mn2O3 particles, which reduces the content of active adsorbed oxygen. This reduction impedes the formation of active bridged nitrates in the aged catalysts and disrupts the SCR pathway through the interaction between bridged nitrates and NH4+ on the composite catalysts. Despite these challenges, some adsorbed oxygen remains on the Mn2O3/Cu-SSZ-39 after aging, ensuring that the aged composite catalyst still exhibits higher activity than the fresh Cu-SSZ-39 catalyst. This observation suggests that there is potential for the application of Mn2O3/Cu-SSZ-39 in practical scenarios.