Insights into Nb doping effects on the catalytic activity and SO2 tolerance of Mn–Cu/BCN catalyst for low-temperature NH3-SCR reaction

Biochar-based supported denitration catalysts have shown tremendous potential in reducing NOx, while improving low-temperature NH3-SCR catalytic activity and SO2 tolerance still faces great challenges. In this work, Mn7–Cu3/BCN and Mn7–Cu3-Nbx/BCN catalysts were prepared by one-step wet impregnation. The enhanced effect of Nb doping on the catalytic performance and SO2 tolerance over the Mn7–Cu3/BCN catalyst was evaluated in the temperature range of 75–275 °C. The denitrification activity test showed that the introduction of an appropriate amount of Nb increased the catalytic activity and N2 selectivity of the catalyst. The NO conversion of Mn7–Cu3–Nb0.05/BCN with an optimum doping ratio of 0.05 wt% Nb was higher than 94% at 150–275 °C. The characterization results indicated that the introduction of Nb enhanced the interaction between the active components MnOx and CuOx, accelerated the electron transfer between elements, and thus improved the Mn4+/Mnn+ and Oα/(Oα+Oβ+Oγ) proportions and redox performance. On the other hand, Nb modification increased the number of weakly acidic sites, which was beneficial for the adsorption and activation of the reducing agent NH3 under low-temperature conditions. Meanwhile, Nb could significantly improve the SO2 poisoning resistance of the Mn7–Cu3/BCN–S catalyst when SO2 was added to the reaction system. The NO conversion of Mn7–Cu3–Nb0.05/BCN remained above 75% after a 13.5 h reaction under 100 ppm SO2 and 5 vol% H2O at 225 °C. By combining experimental characterization results with DFT calculation results, we effectively confirmed that Mn7–Cu3–Nb0.05/BCN had good sulfur resistance, mainly because Nb could effectively inhibit the formation of manganese sulfate and promote the decomposition of ammonium bisulfate. © 2023