Design Strategy of the MnO<i>x</i> Catalyst for SCR of NO with NH<sub>3</sub>: Mechanism of Lead Poisoning and Improvement Method
Hongli Wu, Weizao Liu, Ya Liang, Qingcai Liu
Abstract
The conventional Mn-based catalysts suffer from lead toxicity and require other transition-metal oxides to enhance their resistance in the selective catalytic reduction of NO x with ammonia (NH 3 -SCR). Herein, we found that the incorporation of inert silica into pure MnO x effectively improved the Pb resistance. The NO x conversion of the MnO x -SiO 2 -Pb catalyst was nearly 55% higher than that of the MnO x -Pb catalyst, exhibiting enhanced activity at lower temperatures (150–225 °C). To reveal the essential roles at the molecular level, the types and numbers of surface acidity, nitrate species, and catalytic cycle were established through experimental analysis and theoretical calculations of catalysts. The presence of PbCl 2 occupied the active Mn sites, resulting in an obvious decline in the Brønsted acid sites (B-NH 4 + ) and the oxidation performance, and the NH 3 -SCR cycle was energetically less favorable on the MnO x -Pb catalyst. Conversely, SiO 2 played a crucial role in preserving the activity of Mn sites on the MnO x -SiO 2 -Pb catalyst by preferentially bonding with PbCl 2, generating more active intermediates. Significantly, this work provided mechanistic insights into the role of SiO 2 in regulating the surface acidity, oxidation performance, and stability of active Mn sites, which is helpful for the design of Mn-based catalysts with high Pb resistance for the NH 3 -SCR reaction.