Insight Into the Origins of N₂O Byproduct on Confinement Structure TiO₂/MnSm Catalyst Through Sulfation Pre-Treatment for Low-Temperature NH₃-SCR Reaction

Abstract

Mn-based catalysts are the most promising catalysts for low-temperature NH₃-SCR, but improving N₂ selectivity still faces great challenges. Herein, the tubular structure TiO₂–SO₄²⁻/MnSm assembled from nanosheets was developed, which exhibited superior NO removal efficiency and outstanding N₂ selectivity over a wide operation temperature window in NH₃-SCR. It was experimentally proven that sulfation treatment disturbs the lattice of TiO₂ to effectively promote the generation of oxygen vacancies and raise the proportion of weak acid sites. In addition, Sm modification greatly improved the dispersion of active species and enhanced the metal–support interaction, which promoted the interfacial electron transfer to modulate the activation capacity of NH₃ to reduce the generation of N₂O. Importantly, DFT calculations and in situ DRIFTS revealed that the generation of N₂O originated from the over-oxidation of NH₃ and non-selective catalytic reduction via E–R or L–H mechanism, which required higher Gibbs free energy on catalyst TiO₂–SO₄²⁻/MnSm. This work highlights a new insight into improving the N₂ selectivity of Mn-based catalysts in NH₃-SCR.

Keywords

N₂ selectivity / Sm modification / strong metal-support interaction / sulfation treatment

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