Effect of Hydrothermal Aging Treatment on Decomposition of NO by Cu-ZSM-5 and Modified Mechanism of Doping Ce against This Influence.

Abstract

Cu-ZSM-5 and Ce-doped Cu-Ce-ZSM-5 samples were prepared by liquid-phase ion exchange method. The two catalysts were subjected to hydrothermal aging treatment in the simulated flue gas of a coal-fired power station at an ageing temperature of 650–850 °C. The denitration experiment found that the activity of the aged Cu-ZSM-5 was 19.6% to 41% lower than that of the fresh Cu-ZSM-5 at the optimal decomposition temperature of NO at 550 °C, while the aged Cu-Ce-ZSM-5 had only a 14.8% to 31.5% reduction in activity than the fresh Cu-Ce-ZSM-5. The samples were characterized by XRD, BET, H2-TPR, XPS, NO-TPD, etc. The results showed that hydrothermal aging treatment leads to the dealumination of the ZSM-5 framework and reduces the specific surface area and pore volume of the micropore in the sample. It also exacerbates the isolated Cu2+, and the active center {Cu2+-O2−-Cu2+}2+ dimers migrate towards the sample surface and form inactive CuO. Doping with Ce can promote the dispersion of Cu(OH)+, which was the precursor of {Cu2+-O2−-Cu2+}2+. Ce3+ can preferentially occupy the less active bridged hydroxyl exchange sites, so that copper ions occupy the more active aluminum hydroxyl sites, thereby inhibiting the migration of active centers.