Redox ability dependent SO2 tolerance for low-temperature NH3-SCR of MnO2@MeOX (Me = Ti, Ce, Cu) catalysts

Elucidating the deposition behavior of sulfates on catalysts of low-temperature ammonia-assisted selective catalytic reduction (NH3-SCR) helps improve their SO2 tolerance and applicability. Therefore, this study aimed to explore the impact of the redox properties of low-temperature NH3-SCR catalysts on their catalytic activity and SO2 tolerance. Oxidizing Mn@Ce, neutral Mn@Ti, and reducing Mn@Cu catalysts were prepared, and their NH3-SCR activities and SO2 tolerances were evaluated. Subsequently, the characteristics of the catalyst poisoned by SO2 over time and the deposition behavior of sulfates on the catalyst were analyzed to determine the reaction pathway between SO2 and the NH3-SCR catalyst. The SO2 tolerance of the catalysts decreased in the following order: oxidizing Mn@Ce > neutral Mn@Ti > reducing Mn@Cu. Combined with the characteristic results, we found that the amount of shell-metal sulfate increased with SO2 poisoning time, indicating it was the dominant factor in catalyst deactivation. Specifically, the amount of shell-metal sulfate followed the order Mn@Cu-S12 (31.4 µmol) > Mn@Ti-S12 (24.9 µmol) > Mn@Ce-S12 (9.5 µmol). Additionally, the increasing SO42− ratio from Mn@Me-S4 to Mn@Me-S12 followed the order Mn@Cu (6.7%) > Mn@Ti (4.4%) > Mn@Ce (1.7%), implying that the reduction of Mn@Cu favors chemical SO2 poisoning pathway and facilitates the deposition of copper sulfate. In contrast, Mn@Ce with its strong oxidation properties, is beneficial for inhibiting the chemical poisoning pathway of SO2 and alleviating the deposition of cerium sulfate. Consequently, this study demonstrates that the redox ability of catalyst regulates the SO2 poisoning pathways, aiding the development of low-temperature NH3-SCR catalysts with high SO2 tolerance. © 2024 Elsevier B.V.