Facile H2O-Contributed O2 Activation Strategy over Mn-Based SCR Catalysts to Counteract SO2 Poisoning

Environ Sci Technol. 2023 Oct 3;57(39):14737-14746. doi: 10.1021/acs.est.3c04314. Epub 2023 Sep 22.

Abstract

Mn-based catalysts preferred in low-temperature selective catalytic reduction (SCR) are susceptible to SO2 poisoning. The stubborn sulfates make insufficient O2 activation and result in deficient reactive oxygen species (ROS) for activating reaction molecules. H2O has long been regarded as an accomplice to SO2, hastening catalyst deactivation. However, such a negative impression of the SCR reaction was reversed by our recent research. Here, we reported a H2O contribution over Mn-based SCR catalysts to counteract SO2 poisoning through accessible O2 activation, in which O2 was synergistically activated with H2O to generate ROS for less deactivation and more expected regeneration. The resulting ROS benefited from the energetically favorable route supported by water-induced Ea reduction and was actively involved in the NH3 activation and NO oxidation process. Besides, ROS maintained high stability over the SO2 + H2O-deactivated γ-MnO2 catalyst throughout the mild thermal treatment, achieving complete regeneration of its own NO disposal ability. This strategy was proven to be universally applicable to other Mn-based catalysts.

Keywords: H2O promotion; Mn-based catalysts; NH3-SCR; O2 activation; SO2 resistance.