Superior Oxidative Dehydrogenation Performance toward NH3 Determines the Excellent Low-Temperature NH3-SCR Activity of Mn-Based Catalysts

Mn-based oxides exhibit outstanding low-temperature activity for the selective catalytic reduction of NOx with NH3 (NH3-SCR) compared with other catalysts. However, the underlying principle responsible for the excellent low-temperature activity is not yet clear. Here, the atomic-level mechanism and activity-limiting factor in the NH3-SCR process over Mn-, Fe-, and Ce-based oxide catalysts are elucidated by a combination of first-principles calculations and experimental measurements. We found that the superior oxidative dehydrogenation performance toward NH3 of Mn-based catalysts reduces the energy barriers for the activation of NH3 and the formation of the key intermediate NH2NO, which is the rate-determining step in NH3-SCR over these oxide catalysts. The findings of this study advance the understanding of the working principle of Mn-based SCR catalysts and provide a fundamental basis for the development of future generation SCR catalysts with excellent low-temperature activity.