Abstract
Abstract The impact of SO2 poisoning on Cu-SAPO-18 physicochemical properties and its NH3-SCR reaction mechanism was investigated. After exposing Cu-SAPO-18 to SO2+O2 for 40 min, the sulfite and sulfate species were detected on Cu-SAPO-18 surface, which caused a small decrease in BET surface area and micropore volume, the increase in NH3 storage and the deactivation of some isolated Cu2+ sites. These could be interpreted by the slight micropore blocking, interaction between sulfates and NH3 forming new NH4+ species and the formation of Cu-sulfate, respectively. Additionally, it was observed that isolated Cu2+ ions in pear-shaped cavity of AEI structure, which are beneficial to good low-temperature deNOx activity, were more severely poisoned by SO2 than Cu2+ in the double 6-membered ring (D6R). Accordingly, the NH3-SCR activity below 350 °C was restrained by SO2. Moreover, the in-situ DRIFTS results indicate that Cu-SAPO-18 catalyzed NH3-SCR reaction predominantly proceeds through Langmuir−Hinshelwood (L−H) mechanism at low temperature. SO2 poisoning inhibited the adsorption of NO + O2 and NH3 on Cu2+ sites, thereby decreasing the formation of Cu−NOx and Cu−NH3 intermediates, evidently, the L−H mechanism was suppressed by SO2. Interestingly, the deactivated Cu-SAPO-18 could be regenerated under SCR gas at 550 °C and resumed at least most NH3-SCR activity.
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